m emb ran es Article C h a r a c t e r i z a t i o n a n d A s s e s s m e n t o f a N o v e l P l a t e a n d F r a m e M D M o d u l e f o r S i n g l e P a s s W a s t e w a t e r C o n c e n t r a t i o n – F E E D G a p A i r G a p M e m b r a n e D i s t i l l a t i o n Rebecca Schwantes 1,2,3, * , Jakob Seger 4 , Lorenz Bauer 1 , Daniel W inter 2 , T obias Hogen 4 , Joachim Koschikowski 2 and Sven-Uwe Geißen 4 1 SolarSpring GmbH, 79114 Freibur g, Germany 2 Fraunhofer Institute for Solar Energy Systems, 79110 Fr eiburg, Germany 3 Institute of Power Engineering, T echnische Universität Dr esden, 01062 Dresden, Germany 4 Department of Environmental T echnology , T echnische Universität Berlin, 10623 Berlin, Germany * Correspondence: r [email protected] Received: 15 August 2019; Accepted: 2 September 2019; Published: 6 September 2019 Abstract: Membrane distillation (MD) is an up and coming technology for concentration and separation on the ver ge of reaching commer cialization. One of the r emaining boundaries is the lack of available full-scale MD modules and systems suitable to meet the requir ements of potential industrial applications. In this work a new type of feed gap air gap MD (FGAGMD) plate and frame module is intr oduced, designed and characterized with tap water and NaCl–H 2 O solution. The main feature of the new channel configuration is the separation of the heating and cooling channel fr om the feed channel, enabling a very high recovery ratio in a single pass. Key performance indicators (KPIs) such as flux, gained output ratio (GOR), r ecovery ratio and thermal e ffi ciency ar e used to analyze the performance of the novel module concept within this work. A r ecovery rate of 93% was r eached with tap water and between 32–53% with salt solutions ranging between 117 and 214 g NaCl / kg solution with this particular pr ototype module. Other than recovery ratio, the KPIs of the FGAGMD ar e similar to those of an air gap membrane distillation (AGMD) channel configuration. From the experimental r esults, furthermore, a new MD KPI was defined as the ratio of heating and cooling flow to feed flow . This R F ratio can be used for optimization of the module design and e ffi ciency . Keywords: distillation; high r ecovery rate; brine concentration; zer o liquid dischar ge; membrane distillation module; wastewater concentration; r esour ce recovery 1. Introduction Membrane distillation (MD) has drawn incr easing interest in the last 10 years fr om both academia and applicational parties. Beginning with a wide range of basic testing of various solutions [ 1 – 6 ] and the establishment of thermodynamic pr ocess understanding and modelling [ 7 – 9 ], the state of r esear ch has gradually shifted towar ds a more applied focus, bringing forth mor e advances in fields of bench and pilot scale trials, membrane testing [ 10 , 11 ] and investigations on membrane hydrophobicity as well as the r egeneration of such [ 12 – 19 ]. An increase in modelling, tar geted on module and system or even hybrid system scenarios [ 20 , 21 ] together with tecno-economic calculations for industrial applications [ 22 , 23 ] can also be observed. Overall, a shift of perception is gradually taking place in which MD is no longer seen as strongly as a possible substitute for seawater r everse osmosis (SWRO), but its potential as a pr ocess step in brine or wastewater concentration and recycling is being unfolded; this is especially valid in cases wher e r everse osmosis (RO) reaches its functional boundaries due to high osmotic pr essur e di ff erences. MD is also being adopted in other applications e.g., in the Membranes 2019 , 9 , 118; doi:10.3390 / membranes9090118 www .mdpi.com / journal / membranes Membranes 2019 , 9 , 118 2 of 28 pharmaceutical industry or food industry because it can be operated at ambient pr essur e and with low temperatur es [ 24 – 26 ]. Despite these incr easingly practical advances, MD is not fully commer cialized yet and some of the r easons r epeatedly given ar e the lack of full-scale MD modules, high specific thermal ener gy consumption, low r ecovery rate and a limited variety of available specialized membranes [ 27 , 28 ]. For example, the r egeneration of membrane hydrophobicity in situ and the avoidance of membrane wetting altogether has not yet br ought forth a universal strategy for commer cial implementation in flat sheet MD modules on a large scale, especially when dealing with high salinity feed solutions—although incr easingly tar geted by resear ch in the last few years [ 29 , 30 ]. However , promising r esults have been achieved for specific applications using brines between 1–19% and using por ous fluorosiloxane-coated polypr opylene hollow fibers [ 31 , 32 ]. In addition, technology requir ements in industrial applications can be di ff erent than those pr esent during the technology development conducted at a time when solar -power ed seawater desalination was still the main goal of many MD resear chers and developers. W ith this in mind, and based on the pr evious experience, new adaptations to MD modules and systems ar e necessary in conjunction with piloting in the r elevant industry . Such an opportunity was cr eated by the HighCon pr oject, placed within the funding program W avE–“Future-oriented T echnologies and Concepts to Increase W ater A vailability by W ater Reuse and Desalination” [ 30 ]. The pr ogram was launched by the German Federal Ministry of Education and Resear ch in order to facilitate the adoption of mor e comprehensive and ecofriendly wastewater tr eatment and internal r euse of resour ces in the industry . The project is coor dinated by the T echnische Universität Berlin, Germany . W ithin HighCon, the goal is to recover r esour ces fr om concentrates generated by r ecycling of industrial wastewater at two di ff er ent pilot sites. Membrane distillation was r epr esented by the company SolarSpring GmbH and the Fraunhofer Institute for Solar Ener gy Systems within the consortium. During the pr oject, a zero liquid dischar ge process chain was developed and piloted, based on a chain of membrane technologies and a humidification-dehumidification (HDH) crystallization step as the final stage. Due to the necessity to concentrate the pr etr eated saline wastewater to a near saturation concentration level in the MD system for subsequent crystallization, a redesign of the MD module and system was carried out and then put into practice in a full-scale prototype. The thr ee main goals to be achieved with the new concept ar e: (I) Implementing a plate and frame module design with r eplaceable inner parts; (II) Minimization of the number of components in contact with the highly corr osive feed solution; (III) Enabling of a single pass r ecovery rate high enough to operate the MD stage as a one- step process. These design criteria apply to almost any industrial pr ocess in which highly corr osive or chemically aggr essive or toxic compounds are pr esent in the feed solution and the concentration increase should be high. So far , in the existing MD channel configurations that are based on sensible heat r ecovery and using flat sheet membranes, the unification of points (I)–(III) were not possible on a full scale and is consider ed a drawback of the technology . Also, the r eplacement of inner parts is not possible per se in any module type in which a r esin potting is used for sealing of the material layers. Low module r ecovery rates also mean that to achieve a high incr ease in concentration, the feed must be cir culated in a batch mode or pr ocessed by a serial cascade of modules [ 33 ]. This r equires commer cially available heat exchangers and pumps that ar e chemically resistant to the feed solution to be tr eated. In this work a new module concept is pr esented under the name of feed gap air gap membrane distillation (FGAGMD) which incorporates the solution to r equir ements (I)–(III). Fundamentally , it is a derivation of air gap membrane distillation (AGMD) [ 34 , 35 ], however the feed and the permeate solution are separated fr om the heating and cooling solution by addition of an extra channel. Pr ecise details on the configuration ar e pr ovided in Sections 2.1 and 2.2 . Furthermor e, the new FGAGMD module was constructed and characterized within the HighCon pr oject. A comprehensive description on the pilot Membranes 2019 , 9 , 118 3 of 28 system set-up and experimental configuration is given in Section 2.3 . Full characterization data for tap water and artificial NaCl–H 2 O solution with a salinity up to 214 g NaCl / kg is provided in this work and discussed in the r esults Section 3 . Regar ding the topic of specific thermal ener gy consumption in MD as such, there is still a lack of consensus in publications to pr ovide the key performance indicators necessary to pr operly evaluate the entir e performance of the pr ocess. As explained in [ 22 ], experiments carried out in small-scale bench testing, ar e often pr esented using flux values without any mention of ener gy consumption [ 33 ], thus giving a misleading impr ession on how future pr ocess optimization needs to be carried out. Simply tar geting a high gained output ratio (GOR) in MD module design will, however , not satisfy the futur e market demands, as it is by natur e of the pr ocess always a trade-o ff with transmembrane flux, the latter r educing with incr easing GOR [ 36 – 38 ]. Thus, developments in MD module and process design should be carried out keeping both in mind as described by [ 22 , 38 ]. The question if to maximize GOR or flux should be evaluated car efully on a case to case basis when it comes to the implementation in the industry . W ithin this work flux, GOR, recovery ratio and thermal e ffi ciency ar e used to gain a compr ehensive understanding of the module performance. 2. Materials and Methods 2.1. Membrane Distillation (MD) Pr ocess and the Evolution of Channel Configurations Membrane distillation is a thermal driven membrane process in which a hydr ophobic, micr opor ous membrane constitutes the vapour space. Only vapours can pass through the membranes, non-volatile substances ar e r ejected. The driving for ce of the process is the e ff ective vapour pr essure di ff er ence across the membrane most commonly pr ovided by a temperatur e di ff er ence. Mass transfer in MD is well investigated [ 9 , 39 ] and can be described as a combination of molecular and Knudsen di ff usion transport mechanisms. Heat transfer in MD is characterized by a combination of latent heat and conductive heat transfer and is sensitive to many parameters such as physical membrane properties, spacer selection and operational parameters [ 40 ]. Since the early days of MD [ 41 ], the possible MD channel configurations and pr ocess designs have evolved in several di ff erent dir ections [ 42 – 45 ]. One type of MD system, commercially established by the company memsys [ 46 ], is a combined thermal and vacuum driven pr ocess named VMEMD [ 47 ]. Essentially , it repr esents the process commonly known as multi-e ff ect distillation (MED) equivalent of MD. In this variant the latent heat is recover ed and passed on fr om stage to stage. When talking about plate and frame modules in this work however , the focus will be on the MD pr ocess variants in which sensible heat is r ecovered to incr ease the e ffi ciency , thus r epresenting a multi-stage flash (MSF) type of heat r ecovery principle if thought of in terms of state-of-the-art evaporation technology . In the following, new derivations of MD channel configurations ar e intr oduced. An overview of the commonly known configurations dir ect contact membrane distillation (DCMD) and AGMD [ 48 ], as well as the new configurations feed gap membrane distillation (FGMD) and FGAGMD is pr ovided in Figur e 1 . Membranes 2019 , 9 , 118 4 of 28 Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 4 of 30 Figure 1. Basic channel configurations direct contact membrane d i s t illation (DCMD) and air gap membrane distillat i on (A GM D) and deri ve d “Feed gap” variant feed gap membrane dist illat i on (F GMD) an d f e ed g a p air g a p MD (F GA GM D). The DCMD is the simplest MD config ur ation in whic h a ho t feed solution flow s on one side and the cooled permeate flows on th e o t her side o f the microporous m e mbrane in c o unter c u rren t. Due to th e tem p e r at ure -ind u ce d v a p o ur p r e ssur e gr ad ien t , v a p o ur is tr ansp or ted thr o ugh the m e m b rane pores from th e hot to the c o ld side of th e membrane which then c o ndenses on enter i ng the permeate stre am. An a d vant ag e of t h is con fig ur at ion i s th e hi g h fl ux d u e t o the lo w the r mal b a rr ier o f only the membrane m a terial enab ling high fl ux and therma l eff i cienc y a t l o w sa lin it ies [3 6] . Howeve r, the frac t i on o f co nduct i ve hea t p a s s ed thro ugh the m e m b rane is al so com p arab ly higher l e ad in g to a potent ia ll y lo wer therma l eff i cienc y in module s w i t h si gni fic an t heat recove r y and especi al ly a t higher salinities above 100 g NaCl/k g. T h ere is eno u g h evidenc e in rese arch to ac knowled g e th at th e qu al it y of dis t ill a t e c a n, fur t hermore, be c o mpromi sed by so calle d w e tting pheno m ena an d th at th ese phenomena are enh a nced when there is liquid on bo th sides of t h e membra ne [14 , 4 9 ]. In DCMD t h is i s u n a v oi da ble pe r s e u n d mu s t , t h e r ef or e , be consid ered a disad v antage . Ano t her sy stem -r elated drawb a ck is the req u i r em ent of an ad dit i on al he at exch anger i n order to re cover he at fr om the condenser o u tle t fo r pre-he ating o f the fe ed. In su mm a r y, DCMD is very popul a r in ac adem ia f o r it s sim p l i ci ty an d high f l ux , b u t h a s l i m i t a t i ons when it com e s to u s e in th e in d u s t ry and is not as com m o nly ap p lied on a f u l l sc al e as e . g. , AG MD or PG MD [ 5 0– 5 4 ]. The conf igu r at ion second from the lef t i n Error! R e f e renc e so urc e not found . is AGMD. In th is va ria n t, a t h in pol y mer fi lm sepa ra t e s the di st il lat e cha nnel f r om the cool a n t . Thi s al so ena b les t h e direc t in tern al r e covery of heat inside the modu le, since the feed so lution c a n th ereby be used as coolan t w i tho u t. The addi t i onal a i r g a p i n AG MD al so provides a h i gher th ermal insulation between the ch anne ls. This r educe s the ove r all he at tran sfer , th us lower i ng the flux compared to DCM D but it a l so re duc e s the fr ac ti on of cond u c tiv e he at tr ans f er which i s no t us ed for ev ap ora t ion. A com p rehensi v e com p ar iso n of the two var i an ts DC MD and AG MD i s given b y [4 8] . At higher sa lin it ies , DC MD can be more sens i t ive t o the impac t of vapo ur pre ssur e red u ct i o n [2 2 ] un les s thic ker membranes are used in which case the th icker m e m b rane s u b s t i t u tes th e therm a l in sul a tion p r op ertie s of the a i r gap [ 5 5] . T h e AG ch annel v a ri ant al so giv e s the p o ssib i li ty of ap p l y i ng a v a cuum (v-AGMD ) to reduc e mole cul a r d i f f u s io n res i s t ance s or to us e low - pressu re air s p argin g to en sure a com p lete dr ai nage of the di st il la te, the p o si tiv e ef fect s of wh ich on wett ing ar e r e ported in [ 4 9] . Figure 1. Basic channel configurations direct contact membrane distillation (DCMD) and air gap membrane distillation (AGMD) and derived “Feed gap” variant feed gap membrane distillation (FGMD) and feed gap air gap MD (FGAGMD). The DCMD is the simplest MD configuration in which a hot feed solution flows on one side and the cooled permeate flows on the other side of the micr opor ous membrane in counter curr ent. Due to the temperatur e-induced vapour pr essur e gradient, vapour is transported through the membrane por es fr om the hot to the cold side of the membrane which then condenses on entering the permeate stream. An advantage of this configuration is the high flux due to the low thermal barrier of only the membrane material enabling high flux and thermal e ffi ciency at low salinities [ 36 ]. However , the fraction of conductive heat passed thr ough the membrane is also comparably higher leading to a potentially lower thermal e ffi ciency in modules with significant heat recovery and especially at higher salinities above 100 g NaCl / kg. Ther e is enough evidence in r esear ch to acknowledge that the quality of distillate can, furthermore, be compr omised by so called wetting phenomena and that these phenomena are enhanced when ther e is liquid on both sides of the membrane [ 14 , 49 ]. In DCMD this is unavoidable per se und must, ther efore, be consider ed a disadvantage. Another system-r elated drawback is the r equirement of an additional heat exchanger in or der to recover heat fr om the condenser outlet for pr e-heating of the feed. In summary , DCMD is very popular in academia for its simplicity and high flux, but has limitations when it comes to use in the industry and is not as commonly applied on a full scale as e.g., AGMD or PGMD [ 50 – 54 ]. The configuration second fr om the left in Figure 1 is AGMD. In this variant, a thin polymer film separates the distillate channel from the coolant. This also enables the dir ect internal recovery of heat inside the module, since the feed solution can thereby be used as coolant without. The additional air gap in AGMD also pr ovides a higher thermal insulation between the channels. This r educes the overall heat transfer , thus lowering the flux compared to DCMD but it also r educes the fraction of conductive heat transfer which is not used for evaporation. A comprehensive comparison of the two variants DCMD and AGMD is given by [ 48 ]. At higher salinities, DCMD can be more sensitive to the impact of vapour pr essur e r eduction [ 22 ] unless thicker membranes ar e used in which case the thicker membrane substitutes the thermal insulation pr operties of the air gap [ 55 ]. The AG channel variant also gives the possibility of applying a vacuum (v-AGMD) to reduce molecular di ff usion r esistances or to use low-pr essur e air spar ging to ensur e a complete drainage of the distillate, the positive e ff ects of which on wetting ar e r eported in [ 49 ]. Membranes 2019 , 9 , 118 5 of 28 One featur e of both DCMD and AGMD ar e limitations regar ding the recovery ratio of distillate in a single pass thr ough the module. Since the thermal ener gy for evaporation is carried into the module via the feed str eam on the evaporator side, the permeate output is limited by the sensible heat contained in that str eam. The maximum theoretical r ecovery ratio in a single pass can be calculated by dividing the latent heat of evaporation at the mean pr ocess temperature by the sensible heat supplied be the heating channel. As pr esented in detail by [ 38 ], only approximately 1–8% of the evaporator inlet mass flow can be extracted as permeate in the aforementioned channel configurations. For example, to achieve a concentration incr ease fr om 8% w / w to ~20% w / w of NaCl H 2 O solution, a recovery ratio of 60% would be necessary in or der to r each this goal in a single pass. In order to decouple the thermal ener gy supply fr om the feed stream and over come the limitation of recovery ratio, one possibility is an alternative operation of an AGMD channel set-up. In this so- called FGMD configuration, the feed solution is cir culated through the pr evious air gap and the heating solution is introduced into the former coolant channel which is separated fr om the feed solution by the polymer film. On the cold side of the membrane, the permeate is now circulated as coolant and the vapours condense in that coolant channel in analogy to the DCMD set-up as shown in Figur e 1 . Even though a separation of ener gy supply and feed supply is achieved ther eby , the FGMD configuration still su ff ers from the same drawbacks as the DCMD arrangement r egar ding module internal heat r ecovery , sensitivity towar ds vapour pr essur e reduction and the need for an extra heat exchanger to r ecover the heat from the permeate channel outlet to preheat the feed. Thus, in or der to fulfill all three goals listed in the intr oduction a further modification is needed. FGAGMD describes a variant in which not only the feed solution is separated fr om the heating str eam, but the cooling str eam is also separated fr om the permeate channel. Such a channel arrangement has pr eviously been discussed in conjunction with MD pr ocess integration into heat exchangers by [ 56 , 57 ], but no full scale modules are available to the knowledge of the authors. Due to the addition of the extra second polymer film an additional conductive heat transfer r esistance is added to the thermodynamic r esistance chain. Also, it must be noted that an amount of sensible heat is transported out of the system together with the heated feed solution in the FGMD and FGAGMD channel configurations and is dependent on the feed solution flow rate, physical pr operties and temperature. This must be accounted for in the design of the overall system design of a potential FGMD or FGAGMD module and system, if this exiting heat is to be r ecover ed. Due to the higher suitability of an air gap configuration for the concentration of solutions with a high vapour pressur e reduction compar ed to pure H 2 O and the advantages regar ding the r ecovery of heat inside the module, a FGAGMD channel configuration was chosen for the pilot system and developed within the HighCon project. In addition, goals II and III can only be achieved with a separation of heat supply and feed supply to the module(s). Further advantages of the configuration ar e worth mentioning. The heating and cooling loop can be operated with a single load of water and easily connected directly to available heating and cooling sour ces without interfering with the feed str eam. 2.2. Module Design The goals of MD module design can be outlined as packaging the pr ocess into a device that facilitates a uniform flow distribution in the channels, and reduces ener gy demand, pressur e losses and polarization e ff ects. Cleaning, maintenance and replacement of components should be possible at a r easonable cost. Packing density should be high. All materials used must be mechanically , chemically and thermally adequate for the tar geted application of the module [ 28 ]. A plate and frame FGAGMD module was designed, with an e ff ective channel length of 5.76 m and channel height of 0.72 m. The channel length in an MD module with sensible heat r ecovery determines the temperatur e di ff erence which will be established acr oss the membrane. In opposition to a spiral wound module, the possible channel lengths in a plate and frame type are limited by the length of the individual plates that constitute the channel. The e ff ective channel length can only be a multiple of the single plate length by a serial connection of plates. The single plates are hydraulically connected to Membranes 2019 , 9 , 118 6 of 28 each other via switch plates in or der to achieve a 180 ◦ angle change in flow dir ection at the end of each plate. This way thermodynamic adaptations to specific customer needs can be implemented easily by adding or subtracting a certain number and arrangement of plates. Figur e 2 provides a detailed overview of how the FGAGMD channel configuration was implemented in the pr ototype module. In or der to achieve a minimal heat loss to the ambient, the channels on the r espective outer sides of the module wer e designed to be cold channels. Thus, the only way to package the channel configuration, is to locate the hot channel in the middle of the individual channel set-up. In the schematic in Figure 2 , the channels ar e indicated by the letters H (heating channel), C (cooling channel), D (distillate) and F (feed). The membrane is between each feed (F) and distillate channel (D) and the heating and feed as well as the cooling and distillate channels ar e separated by a thin polypropylene film. The numbers in the channels and plates of the schematic give refer ence to the respective material pr operties in T able 1 . Distillate permeation fr om the feed channels (F) to the distillate channels (D) occurs due to driving for ce temperatur e di ff erence established between the heating channel (H) and the cooling channel (C). The basic thermodynamic principles of MD ar e well published [ 9 , 40 , 58 , 59 ] and will not be r epeated in detail her e. The evaluation of the new module concept will be carried out with use of common key performance indicators pr esented in Section 2.4 . However , the di ff erences of the new FGAGMD to a standar d AGMD configuration should be briefly explained. As presented in Figur e 3 , in FGAGMD an additional conductive r esistance is added through the extra heating channel and polymer film. In AGMD the heating channel is equivalent to the feed channel. The second decisive di ff erence is the heat carried in and out of the system with the feed channel. Depending on the operation parameters, sensible heat leaves the system with the outlet of the feed solution. One method to r ecover this heat is shown in the experimental set-up of the pilot system explained in Section 2.3 . Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 6 of 30 implemen ted easily by ad ding or sub t r a cting a cer t ain number and arr a ngem ent of p l ate s . Error! Ref e rence s o urce n o t f o und. prov ides a d e tailed overview of how th e FGAGMD channel config ur ation was implem ented in the prototype mo du le . In order to achieve a minimal he at loss to the ambien t, the ch annels on the re spec tive o u ter sid e s of the mo dule w e re de signe d to be cold channel s . T h us, th e on ly way to p a c k a g e the ch anne l co n fig ur at io n, i s to loc a te the ho t chann e l in the middle of the indiv i dual c h annel se t-up. In the schem a tic in Error! Ref e rence s o urce n o t f o un d. , the channel s ar e indic a ted by the le t t ers H (hea tin g chan nel) , C (cool i n g channe l), D (di s t i l l a t e ) and F (fee d ). The m e mbrane is be tween e a ch fe ed (F ) and d i stillate ch anne l (D ) and the heating and feed as well a s the co oling an d d i s t i l l a t e ch anne ls are se p a rated by a thin polypropylen e film. The n u mbers in the ch ann e ls and p l a t e s of the sche m a t i c giv e re ference to th e resp ec t i v e m a te ri al p r o p ertie s in Error! R e f e r e nce sourc e n o t foun d. . D i st il la te perme a t i on from th e f eed ch anne ls (F ) to the d i st il la t e channels (D) occurs d u e to dr iving for c e temper ature d i fference established b e tween the h e ating channel (H ) and the coo l ing ch annel (C). Th e ba si c thermod y n a mic pr incip l es of MD ar e wel l publish ed [ 9 , 4 0 , 5 8 , 5 9] an d wi ll n o t be r e peat ed in d e tail here . Th e evaluation of the new module concept will be carr ied o u t with use of c o mmon key p e rform a nce indicator s pre s ente d in Sec t ion 2.4. However, th e di ff erence s o f the new FG AGMD to a s t and a rd AGM D conf ig ura t i o n sho u ld be brief l y explained. A s presen ted in Error! Refer e nc e sour ce no t foun d. , in FG AG MD an a ddi tion al conductive r e sistance is ad ded th rough the ex tr a he ating ch annel and polymer film. In AGM D the heating ch an nel is equivalent to th e feed channel. Th e second d e cisive d i fferenc e is the he at c a rr ied in and o u t of the sy stem with the fe ed ch annel. D e pend ing on th e op era t ion par a meters , sens i b le he at leave s the system w i th the outlet of th e feed so lution . One method to recove r this he at is sho w n in the exper i me ntal set-up o f the pilo t sy stem expla i ned i n S e ct i o n 2 . 3. Figure 2. Detai l ed schemati c o v erview o f the FG AG MD channel configuration. Figure 2. Detailed schematic overview of the FGAGMD channel configuration. Membranes 2019 , 9 , 118 7 of 28 T able 1. Material properties of sub-components used inside the module. No Material Thickness Polymer Approx. Porosity (%) Nominal Pore Diameter ( µ m) 1 + 4 Outer- and switch plate 30 mm Polypropylene (PP) - - 2 + 3 Hot and cold channels 4 mm / 2 mm PP - - 5 Spacer A 2 mm High density Polyethylene (HDPE) 80 - 6 Spacer B 1 mm PP 80 - - Membrane ( + backing) 76 ( + 280) µ m Polytetrafluorethylene (PTFE), (PP) 80 (50) 0.2 - Polymer film 100 µ m PP - - Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 7 of 30 Table 1. Material properties of sub-comp onents used inside the module . No Material Thickness Polymer Appro x . Porosity Nominal Po r e Diameter (%) (µm) 1 + 4 Outer- and switch p l ate 30 mm Polypropylene (PP) - - 2 + 3 Hot and cold channels 4 mm/2 mm PP - - 5 Spacer A 2 mm Hi gh d e ns i t y Poly ethy lene ( H DPE) 80 - 6 Spacer B 1 mm PP 80 - - Membrane (+ backing) 76 (+280) µm Poly tetraflu orethy lene (PTFE), (PP) 80 (50) 0.2 - P o l ymer film 100 µm PP - - Figure 3. Temperature progression al ong the cross- sect ion of the channels . A closer look at the temperature progression from the hot channel to the righ t-side cold chan nel is shown in E rror! Ref e r e n c e sourc e no t found. . As in dicated in Err o r! Ref e rence source n o t fo und. , the thickn ess of the hea t in g channe l i s t w ice th a t of t h e coolin g ch annel since t h e capac i tie s of the tot a l he at ing and coo lin g f l ow sho u ld b e a s s i mi lar as poss ible for the sake o f p r ocess effic i e n cy as shown by [38]. The sche ma also sho w s how the FG AG MD s e t up a dds to the los s o f effec t iv e t e mpera t ure driving force difference at t h e membra ne in terf ace . The los s is expres sed by the difference be tween T H* and T F* an d c a n b e ass i gned d i rect ly to the c o nduct i v e he at loss throu g h th e add i tional film between th e fe ed and the heating so luti on a s well as t h e a d dit i onal t h erma l bounda ry lay e rs in the f eed so lu tion . An a ssemble d modul e i s s h own in Err o r! Ref e rence source no t fo und. 4. Includ ing the outer re info rc em ents , the di m e nsions of the modul e a r e 1 m × 2 m a n d t h e i nner cha nnel di mensi o ns of a si ngl e plate are 0 . 72 m × 1.44 m. The membra ne a r ea of t h e individual modules is ∼ 8 m 2 . This mod u le ′ s she l l was de sign ed to hold a m u ch high er membrane surface than impleme n ted in t h is pil o t sy stem of u p t o 50 m 2 . By par a lle li zin g mu l t iple ch anne ls , the pac k ing densi t y can t h us be improved s i g n ifi c an tl y. Figure 3. T emperature pr ogression along the cr oss-section of the channels. A closer look at the temperatur e progr ession from the hot channel to the right-side cold channel is shown in Figure 3 . As indicated in T able 1 , the thickness of the heating channel is twice that of the cooling channel since the capacities of the total heating and cooling flow should be as similar as possible for the sake of pr ocess e ffi ciency as shown by [ 38 ]. The schema also shows how the FGAGMD set up adds to the loss of e ff ective temperatur e driving for ce di ff erence at the membrane interface. The loss is expr essed by the di ff er ence between T H* and T F* and can be assigned dir ectly to the conductive heat loss thr ough the additional film between the feed and the heating solution as well as the additional thermal boundary layers in the feed solution. An assembled module is shown in Figur e 4 . Including the outer r einforcements, the dimensions of the module are 1 m × 2 m and the inner channel dimensions of a single plate ar e 0.72 m × 1.44 m. The membrane ar ea of the individual modules is ~8 m 2 . This module 0 s shell was designed to hold a much higher membrane surface than implemented in this pilot system of up to 50 m 2 . By parallelizing multiple channels, the packing density can thus be impr oved significantly . Membranes 2019 , 9 , 118 8 of 28 Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 8 of 30 Figure 4. Plat e and frame FGMD module. 2. 3. Ex peri me n t al Se t-U p The p ilo t sys t em consi s t s o f an FG AG M D m o dul e p a ir and a h y dr au lic sy stem and he a t in g o n board. Th e m o dule s are id entic a l tw ins . It is impo rt a n t to no te tha t onl y s y s t em com p onents were consider ed, t h at are free ly av a i l a b l e in t h e m a r k e t an d dec l a r ed as sui t ab le for t h e ap p lic at io n b y the manu fac t u r er . The hea t in g and cool ing loop is oper a t ed in par a l l e l , however , t h e direc t ion of fee d f l o w i s s e r i a l . A s v i s i b l e i n Error! R e f e r e nce sourc e no t f o und . , th e feed flow in m o dule 1 is in par a llel to the coo lin g channe l w h erea s in module 2 i t i s p a r a l l el to the heat ing chan nel. Th is en a b les the recovery o f t h e sens ible h e at le avin g M D 1 in th e sec o nd m o du le MD 2 . For a b e tte r und e rs tan d in g of th e p i lot s e t- up th e f l o w s and com p onents sho w n in Err o r! Ref e r e nce s o urce no t fo und. are describe d as follows: 2. 3. 1 Fe ed Lo op Usin g fee d p u mp P f , fee d solution w i th the properties recorded by sensors T fi1 (te m perature fe ed in MD 1), p fi1 ( p ressure f eed i n MD 1) and C fi1 (cond u ct ivi t y fee d i n MD 1 ) and a vo lume f l o w se t by flow me ter F fi1 is p u m p ed from th e fe ed t a nk into the f i rs t m o d u le (MD 1 ) . Af ter en ter i n g , th e tem p er at ure of the f eed s o lu tion i s inc r eas e d b y the he at ing so lu tion in a cou n ter cur r ent m a nner throu g h the t h in po lymer f ilm. Thu s , a t h ermal dr ivin g force i s es ta b lishe d b e twe e n the fee d so lu tion and the coo l i n g ch annel , w h ich r e su l t s i n a v a p o ur f l ux p a ss ing f r om the feed s o lu tion to the adj a cent dis t i l l a te cha nnel. The r e maind e r of the feed so lu t i on (f low F fo 1 ) , leaves MD 1 at temperat ure T fo 1 and at a cond uct i v i ty o f C fo 1 and ent e rs MD 2 at t e mpera t ure T fi2 wh ich is lower t h an T fo 1 du e to sma ll losse s to the a m b i ent. S i m i l a rl y, in MD 2 a v a p o ur fl u x t o t h e di st il lat e cha nnel is esta bli s hed via t h e temper ature-induced vapo ur pr essure difference . H o w e v e r , i n M D 2 t h e f e e d c h a n n e l f l o w i s c o - curren t to the heat ing ch an nel. It exi t s M D 2 a t tem p e r at ure T fo 2 and conduct i v i ty C fo 2 and flows either b a ck in to the feed so lu t i on tan k or le av e s the sy stem depending o n the position of the con t ro l valve V f . I t is not a b l e th a t the fe e d s t re am is no t ac tiv e ly hea t ed or cool ed b y an y sourc e s o t her th an t h e MD module s. Th is mean s, th at bes i de s the feed tank , feed pump , pip i ng an d sen s ors, no oth e r com p onents requ ire res i s t ance towa rd s high ly con c entr ate d s a l t so lu tion s ( o r p o ten t i a l l y othe r chemicals). Figure 4. Plate and frame FGMD module. 2.3. Experimental Set-Up The pilot system consists of an FGAGMD module pair and a hydraulic system and heating on boar d. The modules ar e identical twins. It is important to note that only system components wer e consider ed, that are fr eely available in the market and declared as suitable for the application by the manufactur er . The heating and cooling loop is operated in parallel, however , the direction of feed flow is serial. As visible in Figure 5 , the feed flow in module 1 is in parallel to the cooling channel wher eas in module 2 it is parallel to the heating channel. This enables the recovery of the sensible heat leaving MD 1 in the second module MD 2. For a better understanding of the pilot set-up the flows and components shown in Figur e 5 ar e described as follows: 2.3.1. Feed Loop Using feed pump P f , feed solution with the properties r ecorded by sensors T fi1 (temperatur e feed in MD 1), p fi1 (pr essure feed in MD 1) and C fi1 (conductivity feed in MD 1) and a volume flow set by flow meter F fi1 is pumped fr om the feed tank into the first module (MD 1). After entering, the temperatur e of the feed solution is incr eased by the heating solution in a counter current manner thr ough the thin polymer film. Thus, a thermal driving force is established between the feed solution and the cooling channel, which results in a vapour flux passing fr om the feed solution to the adjacent distillate channel. The remainder of the feed solution (flow F fo1 ), leaves MD 1 at temperature T fo1 and at a conductivity of C fo1 and enters MD 2 at temperature T fi2 which is lower than T fo1 due to small losses to the ambient. Similarly , in MD 2 a vapour flux to the distillate channel is established via the temperatur e-induced vapour pr essure di ff er ence. However , in MD 2 the feed channel flow is co- curr ent to the heating channel. It exits MD 2 at temperature T fo2 and conductivity C fo2 and flows either back into the feed solution tank or leaves the system depending on the position of the contr ol valve V f . It is notable that the feed str eam is not actively heated or cooled by any sources other than the MD modules. This means, that besides the feed tank, feed pump, piping and sensors, no other components r equir e resistance towar ds highly concentrated salt solutions (or potentially other chemicals). Membranes 2019 , 9 , 118 9 of 28 Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 9 of 30 Figure 5. Sche m a tic of the F G AGMD p ilot sy stem . 2. 3. 2. He at ing and C oolin g Loop The hea t in g a n d coolin g ( H /C) sol u t i on i s pumped fro m the H / C so l u t i on bu ffe r t a nk w i th pu mp P HC contro lle d by flow meter F HC . No spe c ific mater i als need be used here, since th e heat tran sfe r flui d c o n s i s t s o f s o f t e n e d t a p w a t e r . I n c a s e o f a l e a k a g e , a sy stem sh ut-do w n wou l d be triggere d to protec t the non - s a l t wate r re si st a n t com p onen ts in thi s loo p . S i m i l a r l y, p r essu re s e ns or p HCi ha s a s a f e t y func tion . It p r otec ts the m o dule s from overpres sure but also pro v ides a recor ded v a lue fo r the monitoring of pressure during dy n a m i c o p erations. Before en ter i ng both mod u les in par a lle l , the H / C sol u ti on i s cool ed t o a set temperat ure v i a hea t exchanger HEX c ool . T ci1 and T ci2 r e cord the resp ective cooling ch an nel inle t tem p erat ure s o f MD 1 and 2 of wh ich T ci1 is the cont rol senso r. The cooling channel s are sepa ra ted fr om the di st il la te ch anne ls by a thin polymer fi lm. The cool an t ga ins temper ature due to the re covery of he at from the co m b inat ion o f conduct i ve h e at t r an sfe r a n d the laten t he at o f the d i stillate condensing on the f ilm . At the outlet, the temp eratures are r e co rded by T co 1 and T co 2 . The require d ex tern al he at is supp lie d by HEX hot af ter which t h e cool ing s o lu tion becomes t h e hea t i n g solu tion by def i n it ion. In t h e pilot plant, the therm a l ener gy is supplie d by a heating ro d and contro lled to a fixe d te mperature m o nitor ed by sensor T hi1. After the he atin g and cooling sol u t i on h a s ent e re d the modu le , it s temp e r atu r e r e du c e s cons ta ntl y a l ong t h e c h a n ne l d u e to th e he at tr ansfer thro ugh the ho t side p o lymer film in order to pro v ide the proc ess he at to the feed . It ex its the he ating chann e l at temper atures T ho 1 and T ho 2 , be fore f l o w ing b a ck to the H/C bu ffe r t a nk . 2. 3. 3. D i s t i l l a t e The diffusin g water vap o ur en ter s the distil late channel “D ” thro ugh the membrane and condenses on the surface o f the cond enser channe l. T h e distillate d r ain s either through gr avity or is actively d r ain ed by low pre ssur i zed air supplie d by a blower [49]. The volume flow r a te o f th e air is recorded by sensor F air . T h e distillate leave s bo th module s at a m i xed tem p erature T d and a conductivity C d a n d i s c o l l e c t e d i n t h e di st il la t e ta nk . The t a nk ma ss i s c o nt i n u o u s ly r e c o r d ed by t h e ba la nce M d . At a set mass va lue, pump P d i s tr igge re d and the d i s t ill a t e i s p u m p ed e i th er b a c k to the feed tank, fo r operation co ntin uous mo de or dischar g ed to the C I P t a nk to b e used for the p e riodic clean i ng o f th e module alo n gsid e oth e r purposes. Th e CIP sy stem is no t shown in Error! R e f e rence source n ot f o und. as i t s d e t a i l s ar e not r e lev a n t to th i s work, o t her than the f a c t tha t f l u s hin g of the Figure 5. Schematic of the FGAGMD pilot system. 2.3.2. Heating and Cooling Loop The heating and cooling (H / C) solution is pumped fr om the H / C solution bu ff er tank with pump P HC contr olled by flow meter F HC . No specific materials need be used her e, since the heat transfer fluid consists of softened tap water . In case of a leakage, a system shut-down would be triggered to pr otect the non-salt water resistant components in this loop. Similarly , pressur e sensor p HCi has a safety function. It protects the modules fr om overpressur e but also provides a r ecorded value for the monitoring of pr essure during dynamic operations. Befor e entering both modules in parallel, the H / C solution is cooled to a set temperatur e via heat exchanger HEX cool . T ci1 and T ci2 r ecord the r espective cooling channel inlet temperatures of MD 1 and 2 of which T ci1 is the contr ol sensor . The cooling channels ar e separated fr om the distillate channels by a thin polymer film. The coolant gains temperatur e due to the r ecovery of heat fr om the combination of conductive heat transfer and the latent heat of the distillate condensing on the film. At the outlet, the temperatures ar e recor ded by T co1 and T co2 . The r equir ed external heat is supplied by HEX hot after which the cooling solution becomes the heating solution by definition. In the pilot plant, the thermal ener gy is supplied by a heating rod and contr olled to a fixed temperatur e monitor ed by sensor T hi1. After the heating and cooling solution has enter ed the module, its temperature r educes constantly along the channel due to the heat transfer thr ough the hot side polymer film in order to pr ovide the process heat to the feed. It exits the heating channel at temperatur es T ho1 and T ho2 , before flowing back to the H / C bu ff er tank. 2.3.3. Distillate The di ff using water vapour enters the distillate channel “D” through the membrane and condenses on the surface of the condenser channel. The distillate drains either through gravity or is actively drained by low pr essurized air supplied by a blower [ 49 ]. The volume flow rate of the air is recor ded by sensor F air . The distillate leaves both modules at a mixed temperature T d and a conductivity C d and is collected in the distillate tank. The tank mass is continuously r ecorded by the balance M d . At a set mass value, pump P d is trigger ed and the distillate is pumped either back to the feed tank, for operation continuous mode or dischar ged to the CIP tank to be used for the periodic cleaning of the module alongside other purposes. The CIP system is not shown in Figure 5 as its details ar e not Membranes 2019 , 9 , 118 10 of 28 r elevant to this work, other than the fact that flushing of the module is possible in a fully automatic manner . Figure 6 shows an image of the entir e pilot system with indication of the main components. Permanent logging of all sensor values took place during operation to allow a high r esolution of data points and, ther efor e, an adequate accuracy in data analysis. The logging frequency was set to 30 s per datapoint. T able 2 provides a complete overview of sensors and actors used in the system alongside their accuracy (if applicable) as indicated by the manufactur er . T able 2. Sensor and actor list of the pilot system. Component Producer T ype Accuracy Name in Schematic Conductivity meters Jumo, Fulda, Germany CTI500 24VDC ≤ 0.5% of measuring range (0–500 mS / cm) C fi1 , C fo2 Conductivity meter distillate Jumo, Fulda, Germany BlackLine CR-EC ≤ 2% of measuring range (0–5000 µ S / cm) C d V olume flow H / C Krohne, Duisburg, Germany Optiflux 4300C 0.5% of measuring value F H / C V olume flow Feed MIB GmbH, Breisach am Rhein, Germany Flowmax 42i ± 2% of measured value ± 3 mm / s T emperature sensors TC direct, Mönchengladbach, Germany Pt100 Klasse A ± (0.15 + 0.002 × t) all T emperatures Feed pump KNF Neuberger GmbH, Freibur g, Germany PML14169-NF 300 - P f Heating and Cooling pump Dunkermotoren, 79848 Bonndorf im Schwarzwald, Germany BG 65X50 SI - Pressur e sensors Jumo, Fulda, Germany Midas, C18 SW -1,6 1.6% of measuring value p H / Ci , p fi1 PLC Advantech Europe BV , Hilden, Germany 2271G-E1-C20170517 - - Pressurized air pump KNF , Neuberger GmbH, Freibur g, Germany KNF N828 KNE - Blower Balance distillate Soehnle Industrial Solutions GmbH, Backnang, Germany T able balance 1 g for 0–32 kg M d V olume flow air First Sensor AG, Berlin, Germany WT A ± 2% of reading + 0.25% of measuring value F air Heating and cooling pump Harton Anlagentechnik GmbH, Alsdorf, Germany DC 40 / 10BL - P H / Ci Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 11 of 30 Figure 6. Persp e ctive v i ew of t h e pilot sy stem and m o du le s; ( 1 ): ri g wi th pumps , v a lv es an d c o ntrols , ( 2 ): m o du le 1; ( 3 ): m o du le 2; ( 4 ): fee d , concentrate and dist ill ate tank s. 2.4. Ke y Perfor mance In dicato rs For ev aluatio n of the MD process charac teri st ics a n d compa r is on wi th oth e r mod u le s a n d systems, well-estab l ished k e y perform a n c e ind i cators (KPI) w i l l be intro d uced in the fol l owin g and used in th is work. Phys ica l pro p ertie s o f s a l t so lu tion s d i ffer from p u r e H 2 O. Artificial NaCl–H 2 O solutions at differen t salinities w e re used fo r th e c h ar acte risa tio n of the new module type. Thus, a se ries o f measuremen ts was c a rried out to allow a conversion o f th e online m e asured and logged con d uctiv i ty values 𝜎 (mS / cm) in to s a l i n ity v a l u es 𝑆 (g/kg ) . Form ulas (1) and (2) we re derived fo r d i ffe r ent concentration ranges. 𝑺 ( 𝟓 𝝈𝟐𝟏 𝟗 ,𝟓) = 0 ,0017 𝜎 0 ,4309𝜎 5 , 5678 (1 ) 𝑺 (𝝈 𝟐𝟏𝟗,𝟓) = 0 ,0392 𝜎 16, 1099𝜎 1830 ,2558 (2 ) The temper ature and salin ity dependen t values for de nsi t y and sp e c if ic he at cap a ci ty of N a C l –H 2 O solutions we r e der ived fro m the co rrelation s provid e d by [60]. The weigh t measuremen t o f the d i stillate M d (see Erro r ! Refer e nc e s ource not f ou nd. ) over t i me, al lows the ca l c ul at ion o f th e di st il la te f l o w ra te 𝑚 . From th a t , th e tr ansm em b r ane Fl ux 𝑗 (k g/m 2 h ) i n E q u a t i o n ( 3 ) c a n b e c a l c u l a t e d . H e r e , t h e di st il lat e f l o w ra t e 𝑚 is p u t in rel a t i on t o the a c ti ve membra ne surface 𝐴 . F l ux i s w e ll es t a bl ishe d in all membr a ne technolo gies and the r efore allows a good com p ari s on b e twe e n them r e g a rding the specific prod uction o f d i stillate /perme ate. 𝒋 𝒅 = 𝒎 𝒅 𝑨 𝒌𝒈 (𝒎 𝟐 𝒉) (3 ) Another im p o rtan t K P I is the G O R whi c h shows th e relation be tween the the r mal energy amoun t needed for the pure ev aporation pro c ess of the d i stillate (num erator) and the amo u nt o f he at intro duced ex tern ally (den ominator). 𝑮𝑶𝑹 = 𝒎 𝒅 ∗∆ 𝒉 𝒗 𝒎 / ∗𝒄 𝒑 ∗ ( 𝑻 𝒉𝒊 −𝑻 𝒄𝒐 ) [ − ] (4 ) Figure 6. Perspective view of the pilot system and modules; ( 1 ): rig with pumps, valves and controls, ( 2 ): module 1; ( 3 ): module 2; ( 4 ): feed, concentrate and distillate tanks. Membranes 2019 , 9 , 118 11 of 28 2.4. Key Performance Indicators For evaluation of the MD pr ocess characteristics and comparison with other modules and systems, well-established key performance indicators (KPI) will be intr oduced in the following and used in this work. Phys ical p rop erti es of sa lt sol utions di ffer f r om pur e H 2 O. Art ific ial NaCl– H 2 O solu tion s at differ ent sali niti es wer e used for th e char acte risatio n of the n ew mod ule ty pe. Thus, a ser ies of m easu r ements was ca rrie d out to allo w a conv ersion of t he onl ine measu r ed and log ged co nduc tivi ty values σ (mS / cm) into s alin ity va lues S (g / k g). Form ulas ( 1) an d (2) we r e derived f or differ ent co ncen tration r ange s. S ( 5 <σ< 219.5 ) = 0.0017 σ 2 + 0.4309 σ + 5.5678 (1) S ( σ> 219.5 ) = 0.0392 σ 2 + 16.1099 σ + 1830.2558 (2) The temperatur e and salinity dependent values for density and specific heat capacity of NaCl–H 2 O solutions wer e derived fr om the correlations pr ovided by [ 60 ]. The weight measur ement of the distillate M d (see Figur e 5 ) over time, allows the calculation of the distillate flow rate . m d . Fr om that, the tr ansmemb rane F lux j d (kg / m 2 h) in Eq uati on (3) can be c alcu late d. Her e, the dist illa te flow r ate . m d is put i n r elatio n to the a ctiv e membran e surf ace A . Flux is w ell es tablish ed in al l membran e tech nolo gies and th er efor e allow s a good c omparis on bet ween the m r egar ding the s peci fic pr oductio n of dis till ate / per meat e. j d = . m d A " kg ( m 2 h ) # (3) Another important KPI is the GOR which shows the r elation between the thermal ener gy amount needed for the pur e evaporation pr ocess of the distillate (numerator) and the amount of heat introduced externally (denominator). GOR = . m d ∗ ∆ h v . m H / C ∗ c p ∗ ( T hi − T co ) [ − ] (4) wher ein h v (kJ / kg) is the specific evaporation enthalpy , . m H / C (kg / h) is the mass flow rate of the heating and cooling solution, c p , H / C (kJ / kgK) the specific heat capacity the heating and cooling solution, T hi the heating inlet temperatur e and T co the cooling outlet temperatur e. The GOR can be calculated separately for each module by using the matching in- and outlet temperatur es or in total for the module pair using the total distillate pr oduction of both together with the total heat supplied to the modules. W ithin the experiments, distillate mass flow is recor ded via a weight value by a balance. Feed flow however , is r ecor ded as a volume flow . v f . Since the physical properties of NaCl–H 2 O solutions change with incr easing salinity , the calculation of: . m f = . v f ∗ ρ f " kg h # (5) was carried out with density values determined at the r espective feed concentration and 25 ◦ C (temperatur e at point of volume flow measurement) accor ding to [ 60 ]. Based on the same refer ence, specific heat capacity values c p wer e also determined for the r espective concentrations for the mean pr ocess temperatur e T m in the MD module calculated as: T m = ( T ci + T co + T hi + T ho ) 4 [ ◦ C ] (6) wher ein T ci is the temperatur e at the cooling inlet, T co the temperatur e at the cooling outlet and T hi and T ho ar e the temperature s at heating inlet and outlet respectively . T m was typically between 51–52 ◦ C within the experiments conducted for this work. Membranes 2019 , 9 , 118 12 of 28 Thermal e ffi ciency η th given in Equation (7) describes the per centage shar e of latent heat for the liquid vapour phase change of distillate in r elation to the total heat transported thr ough the membrane. η th = . m d · h v . m H / C · c p,H / C · ( T hi − T ho ) · 100 [ % ] (7) Recovery ratio (RR) is the ratio of distillate mass flow rate to H / C flow rate: RR = . m d . m f · 100 [ % ] (8) In Section 3.3 , a new factor R F is intr oduced which describes the ratio of heating and cooling flow to feed flow: R F = . m H / C . m f [ − ] (9) 3. Results 3.1. Performance Characterization with T ap Water In or der to evaluate and compar e the performance of the new module type with the help of KPIs defined in the previous section, measur ements and parameter variations with tap water were carried out. The influence of NaCl–H 2 O solution on the performance is presented in Section 3.2 . The coupling of the module pair , with respect to the serial connection of the feed channels, leads to di ff er ent performance and temperatur e profiles in MD 1 and MD 2. The main reason for this is the intr oduction of additional heat into MD 2, transported by the preheated feed leaving MD 1. Thus, the individual module performance pr ofiles will be analyzed at the beginning of this section, but subsequent evaluation will be carried out for MD 1 and MD 2 combined as a pair , displaying mean values. V olume flow of the heating and cooling loop is given in L / h since it is tap water in all cases and the physical pr operties, especially density , can be assumed to be constant and equal to 1 kg / L. Regar ding the feed flow values, mass flow values wer e derived from the measur ed volume flows using physical pr operties of NaCl solution [ 60 ]. The conductivity of the distillate produced was below 19 µ S / cm during the entir e testing regime with tap water . The pilot system was operated for a total of ~21 weeks with interruptions for the moving of the system fr om the first pilot site in Berlin to the second site in Fr eibur g, Germany . Figur e 7 shows the influence of heating and cooling volume flow on flux and GOR in MD 1. For better legibility , flux is depicted on the left and GOR on the right y-axis. Flux incr eases pr oportionally with the incr ease in H / C volume for all thr ee feed mass flows as a r esult of the higher thermal energy input into the system and subsequent incr ease in bulk temperature di ff er ence. This corr elation is a well-known characteristic of the membrane distillation pr ocess. The flux values ar e not very sensitive towar ds the variation of feed mass flow . However , a certain impact can be observed at 200 and 250 L / h H / C volume flow . When incr easing the feed flow , more heat is lost for MD 1 thr ough the heated feed str eam. Thus, at lower H / C flow rates at which the overall driving force is lower , the impact of that e ff ect is higher , resulting in lo wer flux for higher feed mass flow . GOR values for 40 and 50 kg / h of feed follow the well- known tr end of r educing with incr eased H / C volume flow . This is due to that fact, that the incr ease in driving for ce temperatur e di ff erence is not completely compensated by the incr ease in flux. For a feed mass flow of 50 kg / h the succession of GOR values show that the driving for ce has been r educed over proportionally by the additional heat r equirement to heat the entering feed flow . At 300 L / h H / C flow , the GOR untypically increases slightly due to the now su ffi cient driving for ce supplied by the H / C loop. At this point it could be deducted that the feed flow rate should be as low as possible, in or der to maximize e ffi ciency . For a single module set up, this conclusion would be valid as long as the saturation level of the feed is not reached within the channel after distillate extraction. Membranes 2019 , 9 , 118 13 of 28 As mentioned earlier , in a double module set-up the heat exiting MD 1 with the feed, is recover ed in MD 2 by intr oducing it into the hot side of the module. The feed stream exits MD 1 at appr oximately the mean temperatur e between T hi1 and T co1 (~69–71 ◦ C) depending on the r espective flow pro file. Small losses occur thr ough the piping between the two modules. Feed temperature was ~68–70 ◦ C on entering MD 2. The total distillate output of MD 1 was ~10–14 kg / h depending on the flow pr ofile. This corr esponds with the flux multiplied by the membrane ar ea of 8 m 2 per module. Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 14 of 30 Figure 7. MD 1: influence of H/C volume fl ow on flux and GOR values at different fee d flow rates; tap water; T hi ½ = 80 °C, T ci ½ = 2 5 . Error! R e f e rence s o urc e n o t found . shows fl u x a n d GOR va lu es for MD 2. It mu st be poi n t e d out, th at the feed m a ss flo ws ente ring MD 2 are lo wer th an ind i cated in the naming 30, 40 an d 50 kg/h . These v a lues ind i cate the m a ss flo w at the in le t of MD 1. D u e to the d i s t i l l a te ex tr acte d i n MD 1, they reach MD 2 r educ e d by the respe c tive o u tp ut for each oper ation po int. Err o r! Ref e r e nce source not fo und. sh ows the feed gap mass flo w values for each H / C flo w and FG flo w combinatio n tested with in the ta p wat e r ch ar a c ter i z a t i on m e as urem en ts. Table 3. Feed f l ow rates at the inlet of MD 1, th e inlet of MD 2 and the outl et of MD 2. H/C FG in M1 FG in M2 FG o u t M2 (l/h) (kg/h) (kg/h) (kg/h) 400 30 20.2 9.5 400 40 30.7 19.6 400 50 41.2 30.0 500 30 18.1 4.2 500 40 28.5 14.0 500 50 38.9 24.1 600 30 16.3 2.7 600 40 26.5 9.7 600 50 36.4 19.9 Figure 7. MD 1: influence of H / C volume flow on flux and GOR values at di ff erent feed flow rates; tap water; T hi 1 / 2 = 80 ◦ C, T ci 1 / 2 = 25. Figur e 7 shows flux and GOR values for MD 2. It must be pointed out, that the feed mass flows entering MD 2 ar e lower than indicated in the naming 30, 40 and 50 kg / h. These values indicate the mass flow at the inlet of MD 1. Due to the distillate extracted in MD 1, they r each MD 2 reduced by the r espective output for each operation point. T able 3 shows the feed gap mass flow values for each H / C flow and FG flow combination tested within the tap water characterization measur ements. T able 3. Feed flow rates at the inlet of MD 1, the inlet of MD 2 and the outlet of MD 2. H / C FG in M1 FG in M2 FG out M2 (L / h) (kg / h) (kg / h) (kg / h) 400 30 20.2 9.5 400 40 30.7 19.6 400 50 41.2 30.0 500 30 18.1 4.2 500 40 28.5 14.0 500 50 38.9 24.1 600 30 16.3 2.7 600 40 26.5 9.7 600 50 36.4 19.9 Membranes 2019 , 9 , 118 14 of 28 Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 15 of 30 Figure 8. MD 2: influence of H/C volume fl ow on flux and GOR values at different fee d flow rates; tap water; T hi 1/2 = 80 °C, T ci 1/ 2 = 25. There are so me major differences in the flux and G O R va lue s of M D 2 which are shown in Error! Ref e rence so urce not fo u nd. . To be gi n wit h , t h e over a l l hi g h e r fl ux va lu e s , a r e a di r e ct re s u lt of t h e add i t i ona l the r mal en ergy b e ing s u ppl ied to MD 2 th ro ugh the prehe a te d fe ed com i ng from the o u tlet MD 1. In MD 2 the fl ux is l a rge l y in sens i t ive to va r i a t i o ns of the fee d flow wi th e x ception o f 3 0 kg /h. At 3 0 0 l/h H / C flow and 3 0 kg /h FG inle t f l ow, the f l ux is on ly 1. 7 kg /h m² wh ich i s e q u a l to the val u e at a 250 l/h H/C flow. This phenomenon can be explai ned as fo llow s : In this c a se the di st il la te outpu t is limited by the availabl e feed mass flo w enter i ng M D 2. Since the flux is the h i ghest at 300 l/h H/C flow and 30 k g /h FG flow in MD 1, not e n ough feed is tr ansferred to MD 2 for th e to tal possible flux to be prod uce d . A s shown i n Error! R e f e renc e so urce not f o und . , 1 6 . 3 k g /h are f ed to MD 2 w h ich i s the lowest FG in MD 2 v a lue overall. On ly 2.7 kg /h o f feed leave MD 2. Since th is phenomenon does not occ u r at a FG inle t flow of 40 kg /h, it can be concluded that the o p tim a l fee d flow for max i mized f l u x a t a n H/C f l o w of 600 l/ h l i e s i n between 30 a n d 4 0 kg/ h . The correspondi ng GOR val u e i s a l so sign if ican t l y r educed fo r th at spec if ic opera t ion a l poin t since GO R is ca lcu l ate d in rel a t i on to the ma ss of di st il la te produ c ed. In opposition to MD 1, in MD 2 th e GO R v a lues ar e the high est fo r the highest feed flow of 50 kg/h in ad dition to be be ing over al l h i g h e r t h a n t h e v a l u e s i n M D 1 . A t a f e e d f l o w o f 5 0 k g / h , t h e GOR is ∼ 3 i n MD 2 a n d ∼ 2 in MD 1 at th e s a m e H / C fl ow of 2 0 0 l/h. In an alo g y to th e incre a s e d f l ux , the re ason li e s in the add i t i ona l he at su p p l y ent e rin g MD 2 thro ug h the prehe a ted fee d from MD 1. It incr ea ses th e cool ing flo w out l e t tem p erat ure T co 2 , thus decre asing the de lta T (dTh) on the hot side o f M D 2 . I n c o r r e s p o n d e n c e w i t h E q u a t i o n ( 4 ) a h i g h e r f l u x o r o u t p u t i n t h e n u m e r a t o r a n d a l o w e r temper ature difference be tween T hi and T co in the d e n o mina tor wi ll lead to a hig h er GOR. Thi s eff e ct incre a ses, the higher th e fe ed flow to M D 2 is, d u e to the incre a se i n therm a l cap a ci ty of the fl ow. It h a s been m e ntione d that the temper ature pro f il es o f MD 1 an d MD 2 are affe cted b y the fe ed flow in d i ffer ent deg rees. Error! Ref e r e n c e sourc e no t found. shows the temper ature difference s dTh on the hot an d dTc on the cold side of MD 1 and M D 2 at d i ffere n t H / C vo lume flow s . dT c is th e difference between T ho and T ci of the re spective mo dule. T hi1/2 wa s set a t 80 ° C a n d T ci1/2 at 25 °C. The comparison o f dT v a lues in Error! R e f e rence s o urc e n o t f o und . i s c a rr ied o u t for a feed in le t f l o w of Figure 8. MD 2: influence of H / C volume flow on flux and GOR values at di ff erent feed flow rates; tap water; T hi 1 / 2 = 80 ◦ C, T ci 1 / 2 = 25. Ther e ar e some major di ff erences in the flux and GOR values of MD 2 which are shown in Figur e 8 . T o begin with, the overall higher flux values, are a dir ect r esult of the additional thermal energy being supplied to MD 2 thr ough the preheated feed coming fr om the outlet MD 1. In MD 2 the flux is lar gely insensitive to variations of the feed flow with exception of 30 kg / h. At 300 L / h H / C flow and 30 kg / h FG inlet flow , the flux is only 1.7 kg / h m 2 which is equal to the value at a 250 L / h H / C flow . This phenomenon can be explained as follows: In this case the distillate output is limited by the available feed mass flow entering MD 2. Since the flux is the highest at 300 L / h H / C flow and 30 kg / h FG flow in MD 1, not enough feed is transferr ed to MD 2 for the total possible flux to be pr oduced. As shown in T able 3 , 16.3 kg / h are fed to MD 2 which is the lowest FG in MD 2 value overall. Only 2.7 kg / h of feed leave MD 2. Since this phenomenon does not occur at a FG inlet flow of 40 kg / h, it can be concluded that the optimal feed flow for maximized flux at an H / C flow of 600 L / h lies in between 30 and 40 kg / h. The corr esponding GOR value is also significantly r educed for that specific operational point since GOR is calculated in r elation to the mass of distillate pr oduced. In opposition to MD 1, in MD 2 the GOR values are the highest for the highest feed flow of 50 kg / h in addition to be being overall higher than the values in MD 1. At a feed flow of 50 kg / h, the GOR is ~3 in MD 2 and ~2 in MD 1 at the same H / C flow of 200 L / h. In analogy to the increased flux, the r eason lies in the additional heat supply entering MD 2 thr ough the preheated feed fr om MD 1. It incr eases the cooling flow outlet temperatur e T co2 , thus decr easing the delta T (dTh) on the hot side of MD 2. In corr espondence with Equation (4) a higher flux or output in the numerator and a lower temperature di ff er ence between T hi and T co in the denominator will lead to a higher GOR. This e ff ect incr eases, the higher the feed flow to MD 2 is, due to the incr ease in thermal capacity of the flow . It has been mentioned that the temperatur e pr ofiles of MD 1 and MD 2 ar e a ff ected by the feed flow in di ff er ent degr ees. Figure 9 shows the temperatur e di ff er ences dTh on the hot and dT c on the cold side of MD 1 and MD 2 at di ff erent H / C volume flows. dT c is the di ff er ence between T ho and T ci of the r espective module. T hi 1 / 2 was set at 80 ◦ C and T ci 1 / 2 at 25 ◦ C. The comparison of dT values in Figur e 9 is carried out for a feed inlet flow of 40 kg / h. The dTh MD 1 values are higher than then dT c MD 2 values for both the given flow rates. Heat leaves the system with the feed outlet on the hot side Membranes 2019 , 9 , 118 15 of 28 of MD 1 leading to a decrease in heat r ecovery in the module and subsequently a lower T co1 . Thus, dTh MD 1 is higher than dT MD 2 in which that heat is added to the thermal energy supply coming fr om the heat exchanger HEX hot . T co2 incr eases, r esulting in the lower dTh MD 2 values depicted in the bar chart. Since the heating inlet temperatur e T hi is set at 80 ◦ C, the generally incr eased delta T hot values at 300 L / h ar e r esult of decr ease in cooling outlet temperatur e T co . The hot side delta T ratio of MD 1–MD 2 decr eases fr om 4.4 to 3.3 K. Because a higher flux is generated at this flow rate, the feed flow r eaching MD 2 is lower than at 200 L / h. This results in a dispr oportional relation of the hot side delta T s to one another when the H / C flow rate is increased at the same feed inlet mass flow rate. Opposite e ff ects can be observed regar ding the cold side delta T s. dT c is much lower in MD 1 than in MD 2. On the cold side of the module, T ho1 is decr eased by the additional thermal capacity of the feed entering MD 1 at appr oximately the same temperatur e as T ci . By the time the feed has r eached the outlet of MD 2, the mass flow has so far r educed, that the impact on T ho2 is low . This is shown by the fact that dTh MD 2 and dT c MD 2 are very similar as could be expected e.g., in a counter curr ent heat exchanger . dTh MD 2 is 0.9 K lower than dT c MD 2 at 200 L / h and 0.8 K lower at 300 L / h H / C flow . It has been shown by [ 38 ] that a symmetrical temperatur e pr ofile along the flow channels of MD modules will have a beneficial e ff ect on pr ocess e ffi ciency . This can be achieved by synchr onizing the mass flow capacities in the flow channels. In this new channel configuration however , complexity is added by the mass flow capacity of the feed-baring channel. In MD 1, the capacity of the feed channel ads to that of the cooling channel due to their co-curr ent flow r elation. In MD 2 however , the feed flows co-curr ent to the heating channel making the temperature pr ofiles in MD 1 and MD 2 not only asymmetrical but also unequal, however , with a much lower impact in MD 2 due to the lower feed mass flow . A r eduction in pr ocess e ffi ciency must be expected in comparison to a configuration with parallelized temperatur e pr ofiles as a trade-o ff for the advantages of being able to establish a one- step pr ocess design. Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 16 of 30 40 k g /h . Th e dTh MD 1 v a lue s are h i gh er than then dTc MD 2 v a lues for bo th the g i ven flow r a te s. Heat le aves the system with the feed o u tlet on th e hot side of M D 1 le ad in g to a decre ase in heat recovery in the module and subseque ntly a lower T co 1 . Thus, dT h MD 1 is higher th an dT MD 2 in which th at he at is ad ded to the therm a l ener gy supply coming fro m the he at ex changer HEX ho t . T co 2 i n c r ea s e s, r e su lt i n g i n t h e lowe r d T h MD 2 va lu e s de pi c t ed i n t h e ba r c h a r t . S i nc e t h e he ating i n l e t tem p er at ure T hi is se t a t 8 0 °C, the gen e ra lly inc r ea s ed de lt a T h o t v a l u es at 30 0 l / h are re sul t of decrease in c ooling outle t temper ature T co . The ho t side delta T r a tio of MD 1–MD 2 decre ases from 4. 4 to 3 . 3 K. B e cau s e a hi gh er fl ux is gen e ra ted a t th is flow r a te , the feed f l ow rea c hing MD 2 is lowe r than a t 2 0 0 l / h. This re su lt s in a di sprop o rtion a l re lation of the h o t side delta Ts to one anothe r when the H / C flow rate is incr eased at th e sam e feed inle t m a ss flow rate . Opposite effe cts c a n be observed regarding th e cold sid e de lta Ts. dTc is much lowe r i n MD 1 than in MD 2. On the co ld s i de of th e module, T ho 1 is dec rease d by the ad dition al the r mal cap a city of th e feed enterin g M D 1 at ap p r oxim ate l y the sam e te m p erat ure as T ci . By the time the feed h a s re ached th e outle t of M D 2, the mass flow h a s so far r educ ed, th at th e impact on T ho 2 is low . Thi s is shown by th e fac t tha t dT h MD 2 and dTc MD 2 are very sim i lar as could b e expecte d e.g ., in a coun ter curren t he at e x changer . dT h MD 2 i s 0 . 9 K low e r th an dTc MD 2 at 2 00 l / h and 0 . 8 K l o wer a t 3 0 0 l / h H/C f l ow. I t ha s b een sh own b y [3 8] th at a sy m m e tric al te m p erat ure p r ofi l e along th e flow chann e ls o f MD m o dule s wi ll h a ve a benefic ia l ef fe ct on proce s s eff i cienc y . Th is can be ach i eved by s y nc hroniz ing the mass f l ow ca paci tie s in the flow c h annels. In th is new chann e l con f igur ation however, complexity is added by th e mass flow c a pac i ty of the feed-b a rin g ch annel. In MD 1, th e capac i ty o f the feed chan nel ads to that of th e cooling ch an nel due to the i r co -cu rren t f l ow r e l a t i on. In MD 2 how e ver, the f eed f l ows co-c urr e nt to the he a t ing c h annel m a k i n g the tem p er at ure p r o f i l es in MD 1 and MD 2 not on ly asym m e tr i c al b u t al so uneq u a l, however, wi th a m u ch lo wer imp a ct i n MD 2 due to the lower feed mas s flo w. A reduc t ion in process effic iency m u st be expec t ed in compa r i s on t o a conf igu r a t ion wit h pa ra ll eli z ed tem p er at ure p r ofi l es a s a t r ade - of f for t h e advan t age s o f b e ing ab l e to e s t a b l ish a one - s t ep p r ocess design. Figure 9. Influence of H/C vo lume flow on t e mperature differences in MD 1 and MD 2; 𝒗 𝒇 = 40 kg/h, T hi 1 / 2 = 80 °C, T ci ½ = 25 Figure 9. Influence of H / C volume flow on temperature di ff er ences in MD 1 and MD 2; . v f = 40 kg / h, T hi 1 / 2 = 80 ◦ C, T ci 1 / 2 = 25. Membranes 2019 , 9 , 118 16 of 28 Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 17 of 30 Figure 10 . I n f l u e n c e o f H C v o l u m e f l o w o n F l u x a n d G O R v a l u e s a t v a r i e d f e e d f l o w r a t e s ; M D 1 + MD2 com b in e d ; Tap water; T hi ½ = 80 °C, T ci ½ = 25. Error! R e ference s o urc e n o t f o und . sh ows m e an f l u x and G O R val u es fo r MD 1 and M D 2 combined. To tal output w a s reco rded an d then divi de d by th e to tal membrane ar ea of both mo dule s to de riv e f l ux . S i m i la rly , G O R w a s ca lc ul ate d b y t a k i ng into acco unt the tot a l outp u t and t h e to t a l heat us ed fo r both modu le s. Tot a l H / C flow for both module s i s depict ed on t h e x-ax is . It c a n be observed, that when considering MD 1 and MD 2 as a joined conc ept, th e diffe r e nce between 40 and 50 kg/h feed flow rate is no longer visible since al l sen s ible he at le aving MD 1 w i th the fe ed flow is recovered in MD 2. Thi s is however no t va lid for 3 0 kg/h for rea s ons exp l a i ne d in conj unct i o n wi th Error! Ref e r e nce sourc e no t found . . A ll of the fol l owi n g graphs sh ow combined valu es for M D 1 and MD 2. One of th e m a in r e asons for separ a tin g the he at ing and coolin g flow from th e feed flow, is the possibility o f controllin g th e recovery r a tio of the mod u le independ e ntly of the e n ergy supply . Error! Ref e rence s o urce n o t fou nd. show s th e ach i eved re covery r a tios with tap water as fe ed. Since the recov e ry r a ti o R R i s a r a t i o of d i s t i l l a te o u tp u t to feed input (E q u a t i o n (8 )) , more dis t i l l a te pro d uct i on f r o m t h e s a m e f e e d f l o w r a t e w i l l r e s u l t i n a h i g h er RR. Thus, with increase of H / C flow the RR values also incre a se . As shown in Error! Ref e r e nc e so urc e not foun d. , the distillate flux does no t change sign if ican t l y with ch ange s in fe ed f l ow r a te . Thi s re su l t s in a red u ct i o n of RR for i n creas i ng fee d mas s flow. It shou l d b e p o in ted out, th a t the highes t v a l u e of 9 3 % RR w a s ach i ev ed a t a H / C flow rat e o f 600 l/h and feed flow of 30 k g /h . This value m i g h t even be e x ceedab l e if the aforemen tione d limi t at ions re gard ing di st il la te pro d uc ti on in MD 2 h a d no t occ u rr ed. Therma l ef fi ci ency η th ( E q u a t ion ( 7 )) in dica te s the fr act i on o f l a t e nt he a t in rel a t i on to the t o ta l heat tr an spor ted thro ugh the membrane . Since the inc r ea s e in fl ux i s proport i ona t e to th e inc r e a se in H/C flow, th e η th value s presented in Error! Refer e nce s o urc e n o t f o und . rema in a pproxima t ely constant for H/C flow v a riation. η th wi ll serve as a KPI i n t h e compa r ison wit h a previ o usl y a n a l yz ed spir al wo und module in Se ction 3. 4. Sin c e Error! R e fer e nc e sourc e n o t fo und. sho w s mean v a lu es for both modu les , it is wo rth mention i ng t h at the indiv i dua l va lu es were not ide n tic a l b u t w i t h in ∼ 10% of e a ch o t her . T h e t a p w a ter ch ar ac teri za tion p r es e n ted w i thin t h is sec t ion h a s shown, th at th e Figure 10. Influence of HC volume flow on Flux and GOR values at varied feed flow rates; MD 1 + MD 2 combined; T ap water; T hi 1 / 2 = 80 ◦ C, T ci 1 / 2 = 25. Figur e 10 shows mean flux and GOR values for MD 1 and MD 2 combined. T otal output was r ecor ded and then divided by the total membrane area of both modules to derive flux. Similarly , GOR was calculated by taking into account the total output and the total heat used for both modules. T otal H / C flow for both modules is depicted on the x-axis. It can be observed, that when considering MD 1 and MD 2 as a joined concept, the di ff erence between 40 and 50 kg / h feed flow rate is no longer visible since all sensible heat leaving MD 1 with the feed flow is r ecovered in MD 2. This is however not valid for 30 kg / h for r easons explained in conjunction with Figur e 8 . All of the following graphs show combined values for MD 1 and MD 2. One of the main r easons for separating the heating and cooling flow from the feed flow , is the possibility of contr olling the r ecovery ratio of the module independently of the ener gy supply . Figure 11 shows the achieved r ecovery ratios with tap water as feed. Since the recovery ratio RR is a ratio of distillate output to feed input (Equation (8)), more distillate pr oduction from the same feed flow rate will r esult in a higher RR. Thus, with incr ease of H / C flow the RR values also increase. As shown in Figur e 10 , the distillate flux does not change significantly with changes in feed flow rate. This results in a r eduction of RR for incr easing feed mass flow . It should be pointed out, that the highest value of 93% RR was achieved at a H / C flow rate of 600 L / h and feed flow of 30 kg / h. This value might even be exceedable if the afor ementioned limitations r egar ding distillate pr oduction in MD 2 had not occurr ed. Thermal e ffi ciency η th (Equation (7)) indicates the fraction of latent heat in r elation to the total heat transported thr ough the membrane. Since the increase in flux is pr oportionate to the increase in H / C flow , the η th values pr esented in Figur e 12 r emain approximately constant for H / C flow variation. η th will serve as a KPI in the comparison with a previously analyzed spiral wound module in Section 3.4 . Since Figur e 12 shows mean values for both modules, it is worth mentioning that the individual values wer e not identical but within ~10% of each other . The tap water characterization presented within this section has shown, that the pr oposed concept of a FGAGMD channel configuration with a double module strategy pr ovided the desired operational behavior . In the new concept, the basic KPIs flux Membranes 2019 , 9 , 118 17 of 28 GOR, r ecovery ratio RR and thermal e ffi ciency η th . showed the same dependencies as expected in membrane distillation with a very high incr ease in achievable r ecovery rate. Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 18 of 30 proposed con c ept of a FGA G MD channe l conf ig ura t io n with a dou b le modu le s t rat e gy prov id ed the desir ed oper ational behav i or. In the ne w concept, th e bas i c K P I s fl u x GO R , r e co ve r y rat i o RR a n d therm a l e f ficiency η th . showed the sam e dependencies as expect ed in membrane dist illat i on wit h a very hi gh inc r eas e in ach i e v able r e cover y ra te . Figure 11. Infl uence of H/C v o lume flow on recovery rati o (RR) at differe nt feed flow ra tes; MD1 + MD2 combine d ; tap water; T hi ½ = 80 °C, T ci ½ = 25. Figure 11. Influence of H / C volume flow on recovery ratio (RR) at di ff er ent feed flow rates; MD 1 + MD 2 combined; tap water; T hi 1 / 2 = 80 ◦ C, T ci 1 / 2 = 25. Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 19 of 30 Figure 12. Influence of H/C v o lume flow on thermal efficie n cy η th at differ e nt feed flow rates; MD1 + MD2 combine d , tap water, T hi ½ = 80 °C, T ci ½ = 25. 3.2. Performan c e Chara c teriz a tion with Na Cl Solution Membrane distillation is c a pable o f con c entr at ing so lutions to ne ar sa tur a tion, provided th at crys ta l form a t ion do es no t occur. B e ing an amb i ent p r essure proce ss, limitation s due to e . g., a high osm o tic p o te nti a l of the s o lu tion are n o t an i s s u e. I n MD, howe v e r, th erm a l energy is req u ire d to b r ing ab ou t t h e evap or at io n of th e fe ed solu t i on. W i t h an in cre a si ng amo u nt o f sa lt ions in t h e feed solution, the r e quired ene r g y to evapor ate th e same am ount of d i stillate incre a se s, due to the dec rease in va pour pressure of t h e solut i on. For a given MD sy stem w i th de fined ch anne l geometr y an d fix ed operat ion co ndit ions , th is means th a t f l ux and GO R will d e cre a s e contin uou s l y , the more s a l t ion s are presen t in the feed solution . I t is challeng in g to ach i eve a high GO R i n hypers a lin e brine concentr at ion with MD. Pu blishe d d a t a with fu ll -sc a le modu les i s sca r ce bu t of hi ghest i m port a n ce for ass e ssme n t o f the re a l performanc e of MD techn o logy. Tes t in g and p ilo tin g resu lt s u ch as thos e presented in this work c a nnot and sho u ld no t be co mpared to re sults ach i eve d with tap w a te r or measured in small scale lab equipment. Error! Ref e r e nce so urce no t foun d. sho w s the v a lue trend of flux in correlation with conc entr ate sa lin ity a t an H / C flow r a te of 60 0 l / h and an inle t feed f l ow ra t e of 4 0 kg /h. The s a l i ni ty of the concentr ate at the outlet of MD 2 was se lected fo r de piction on th e x- axis , f l ux and G O R a r e shown on the left an d righ t y-axis respec tive ly. Duri n g these experimen t s the blower , indic a ted in Error! Ref e rence so urce no t fou nd. , wa s op er ate d con t inuo usl y a t an avg. a i r vo lum e f l owr a te o f 1 7 l / h. It has been sho w n by [49] in a stud y w i th an AG MD m o dule , th a t when opera t in g with sa lt so lu tion s, t h e benefi t of opt i ma l dra i ni ng of t h e di sti l l at e i n t h e a i r ga p cha nnel has a signif i c a n t posi ti ve impa ct on t h e di st il lat e qu al it y. A low- pressu re a i r bl ower is an e f f i ci ent m e thod of improving the draining. The di st il la te conduct i vi ty was be low an avg . o f 1 mS /cm du ri ng al l t h e sa lt solu ti on mea s u r ement s . T h e w e l l - k n o w n i m p a c t o f v a p o u r p r e s s u r e r educ t ion [39] can be observed distinc t ly in Error! Ref e rence so urce not fo un d. . B e ginn ing at ∼ 1. 9 kg /h f o r the low e s t sa lin ity , fl ux r educes t o 0. 8 7 k g /h Figure 12. Influence of H / C volume flow on thermal e ffi ciency η th at di ff erent feed flow rates; MD 1 + MD 2 combined, tap water , T hi 1 / 2 = 80 ◦ C, T ci 1 / 2 = 25. Membranes 2019 , 9 , 118 18 of 28 3.2. Performance Characterization with NaCl Solution Membrane distillation is capable of concentrating solutions to near saturation, provided that crystal formation does not occur . Being an ambient pressur e process, limitations due to e.g., a high osmotic potential of the solution ar e not an issue. In MD, however , thermal energy is r equired to bring about the evaporation of the feed solution. W ith an increasing amount of salt ions in the feed solution, the r equir ed energy to evaporate the same amount of distillate incr eases, due to the decrease in vapour pr essur e of the solution. For a given MD system with defined channel geometry and fixed operation conditions, this means that flux and GOR will decr ease continuously , the more salt ions ar e present in the feed solution. It is challenging to achieve a high GOR in hypersaline brine concentration with MD. Published data with full-scale modules is scarce but of highest importance for assessment of the r eal performance of MD technology . T esting and piloting result such as those pr esented in this work cannot and should not be compared to r esults achieved with tap water or measured in small scale lab equipment. Figur e 13 shows the value tr end of flux in correlation with concentrate salinity at an H / C flow rate of 600 L / h and an inlet feed flow rate of 40 kg / h. The salinity of the concentrate at the outlet of MD 2 was selected for depiction on the x-axis, flux and GOR ar e shown on the left and right y-axis respectively . During these experiments the blower , indicated in Figure 5 , was operated continuously at an avg. air volume flowrate of 17 L / h. It has been shown by [ 49 ] in a study with an AGMD module, that when operating with salt solutions, the benefit of optimal draining of the distillate in the air gap channel has a significant positive impact on the distillate quality . A low-pr essure air blower is an e ffi cient method of impr oving the draining. The distillate conductivity was below an avg. of 1 mS / cm during all the salt solution measur ements. The well-known impact of vapour pressur e reduction [ 39 ] can be observed distinctly in Figur e 13 . Beginning at ~1.9 kg / h for the lowest salinity , flux reduces to 0.87 kg / h for the highest outlet salinity of 214 g NaCl / kg. The succession of GOR values is corr esponding to this and pr ovides a range of 1.76–0.78 depending on the concentrate salinity . The decr ease in thermal e ffi ciency η th over salinity is shown in Figur e 14 . The r eduction in vapour pr essur e caused by the increase in dissolved ions in the solution r educes the e ff ective driving force for evaporation. Thus, the ratio of heat used for actual phase change in relation to the total heat transferr ed thr ough the membrane and air gap shifts with incr easing feed salinity . W ith tap water , 67% of the total heat is being used for evaporation. At 214 g NaCl / kg this fraction is r educed to 39%. The r ecovery ratio is furthermor e a ff ected by the r eduction in flux. At the lowest salinity of 1 g NaCl / kg, 76% of the feed going into the inlet of MD 1 is extracted as distillate. This means that 9.6 kg / h exits MD 2 out of the 40 kg / h which enter ed MD 1. At 214 g NaCl / kg, the recovery ratio RR r educed to 32% as a result of the r educed flux. Membranes 2019 , 9 , 118 19 of 28 Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 20 of 30 for the h i ghe s t ou tl et s a lin ity o f 2 1 4 g NaC l /k g. The s u cces s ion o f GO R v a lue s i s co rrespon ding to this and prov ides a ran g e of 1 . 7 6–0 .7 8 dependi n g on the concentrate salinity. The decre ase in th ermal e f ficienc y η th ov er s a l i ni ty is shown in Error! R e f e rence sourc e n o t found. . The r educ t ion in vapour pre s sure caused by th e incr ease in disso lved ions in th e so lution reduce s the e ffec t ive dr ivi n g forc e for evapora t ion. Thus, the ratio of heat used for ac tual phase change in re l a t i on to the tot a l he a t tr a n sferr ed thro ugh the m e m b rane and air g a p shi f t s wi th i n crea si ng f e ed sa li nit y . Wit h ta p wat e r, 6 7 % of t h e t o ta l hea t i s bei n g used f o r eva p orat ion. At 214 g NaC l /k g this frac tion is re duced to 39% . The reco ver y ratio is fur t hermore affec t ed by the re duction in f l ux . At the lowe st s a l i ni t y of 1 g N a Cl / kg, 7 6 % o f th e fee d go ing i n to the inl e t o f MD 1 i s ex tr act ed as di st il l a te . This m e an s t h at 9. 6 kg /h e x its MD 2 ou t o f the 40 k g / h wh ich ent e red MD 1. A t 2 1 4 g NaC l /k g, the recov e ry r a ti o R R re duced to 3 2 % as a r e su lt of the re duced fl ux. Figure 13. Infl uence of concentrate sal i nit y on flux an d GOR ; MD1 + MD2 combin ed; feed inl e t salinity 0.3/55/95/143 g NaCl/kg; 𝒗 𝒇 = 40 kg/h, 𝒗 𝑯/𝑪 = 600 l/h , T hi ½ = 80 °C, T ci ½ = 25 Figure 13. Influence of concentrate salinity on flux and GOR; MD 1 + MD 2 combined; feed inlet salinity 0.3 / 55 / 95 / 143 g NaCl / kg; . v f = 40 kg / h, . v H / C = 600 L / h, T hi 1 / 2 = 80 ◦ C, T ci 1 / 2 = 25. Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 21 of 30 Figure 14. Inf l u e nce of conce n trate salinity on recovery ratio (RR) and t h erm a l efficien cy η th ; MD1 + MD2 combined; Fee d inle t sa linity 0.3/55/95/143 g NaCl/kg; 𝒗 𝒇 = 40 kg/h, 𝒗 𝑯/𝑪 = 600 l/ h, T hi ½ = 80 °C, T ci ½ = 2 5 3. 3. R a ti o of H / C Sol u ti on Fl ow to Fe ed Flo w For a deeper understandin g of the benefits o f th e over all mod u le an d system con c ept some ke y fac t s sho u ld be elabor ated more clo s ely. The go al of the concep t is to ach i eve the desired incre a se in feed solution concentr ation in a sin g le pass process. Th is w a s no t ach i eved in th is p a rtic ular pro t otype system d u e to a r estric t ion in the system s operatio n. T h e H/C flowr a te was limited to 600 l/h, due to t h e ca pa ci ty o f pu mp P H/ C . As es tab l i s hed b y the ev al ua ti on of the tap wa t e r char ac ter i za tion measuremen ts, the r a tio o f heating an d cooling flow rat e to fe ed f l o w ra te h a s a high im p a c t on the recovery ratio. The effect is connec t ed to the prop ortionally h i gher flux pr oduc tion out o f th e same amoun t o f feed flow wh en increasing t h e H/ C f l o w ra te. Thus, a new ra ti o R F is es t a bli s hed (E q u at ion (9 )) , wh ich d e scribe s the q u ot ient o f H/ C mas s flow 𝑚 / to fe ed m a ss flow 𝑚 . E rror! Ref e r e nc e source n o t fo und. depic ts the influence of R F on reco very r a tio RR for three different fe ed salinity levels. The impact of both R F and salinity on recov ery r a tio can now be obser v ed. Line ar fit curve s are used to show the pro g ression o f the recover y r a tio w i th inc r easing R F . T h e re quired R F for a desir ed recov e ry r a tio incr ease s with in creasing feed salin ity . For e x ample, for a require d RR of 50% in a single pass proce ss at an in le t feed concentr ation of 1 g NaCl/kg, R F of ∼ 5 would be s u f fic ient accord ing to the op e r a t in g tem p er a t ur e s of the p ilo t sys t em . A t 14 3 g NaC l / k g inle t conc entr at ion however, the incl ina t ion of the v a l u es is much lowe r a n d a h i ghe r R F would be re quired , tak i n g in to consi derat i o n t h at Na C l –H 2 O sol u t i on is s a tur a ted at ∼ 25 3 g NaC l /k g. Th ese corre l a t i ons are dependent o n the module ’s channel len g th and ar e o n ly va lid for t h is spec if ic module . None t h eles s, the princ i ples for fu tur e mo dule and proc ess des ign re main e q u a l fo r any geome t ry. For a g i ve n in le t feed conc entr ation and a d e si re d fin a l c o ncentr ation, R F must be d e term ined in order to achieve the r e q u i r e d r e c o v e r y r a t i o . C e r t a i n b o u n d a r y c o n d i t i o n s m u s t a l s o b e c o n s i d e r e d . I n o r d e r t o s u s t a i n overall e f ficie n cy, the feed flow canno t be lowered to a value that do es not supp ly a suffic ien t amount of fe ed to MD 2. The neg a t i ve eff e ct s on GOR and the r mal ef fic ienc y were ana l y z ed in S e ct io n 3. 1. In add i tion, a safe ty m a rg in to preven t satur a tion of the so lution in MD 2 sho u ld be ad de d to the minimum feed flow ra te. Figure 14. Influence of concentrate salinity on recovery ratio (RR) and thermal e ffi ciency η th ; MD 1 + MD 2 combined; Feed inlet salinity 0.3 / 55 / 95 / 143 g NaCl / kg; . v f = 40 kg / h, . v H / C = 600 L / h , T hi 1 / 2 = 80 ◦ C, T ci 1 / 2 = 25. 3.3. Ratio of H / C Solution Flow to Feed Flow For a deeper understanding of the benefits of the overall module and system concept some key facts should be elaborated mor e closely . The goal of the concept is to achieve the desired incr ease in feed solution concentration in a single pass pr ocess. This was not achieved in this particular Membranes 2019 , 9 , 118 20 of 28 pr ototype system due to a r estriction in the systems operation. The H / C flowrate was limited to 600 L / h, due to the capacity of pump P H / C . As established by the evaluation of the tap water characterization measur ements, the ratio of heating and cooling flow rate to feed flow rate has a high impact on the r ecovery ratio. The e ff ect is connected to the proportionally higher flux pr oduction out of the same amount of feed flow when increasing the H / C flow rate. Thus, a new ratio R F is established (Equation (9)), which describes the quotient of H / C mass flow . m H / C to feed mass flow . m f . Figure 15 depicts the influence of R F on r ecovery ratio RR for three di ff er ent feed salinity levels. The impact of both R F and salinity on r ecovery ratio can now be observed. Linear fit curves are used to show the pr ogr ession of the recovery ratio with incr easing R F . The r equir ed R F for a desir ed recovery ratio incr eases with incr easing feed salinity . For example, for a r equir ed RR of 50% in a single pass pr ocess at an inlet feed concentration of 1 g NaCl / kg, R F of ~5 would be su ffi cient accor ding to the operating temperatur es of the pilot system. At 143 g NaCl / kg inlet concentration however , the inclination of the values is much lower and a higher R F would be r equired, taking into consideration that NaCl–H 2 O solution is saturated at ~253 g NaCl / kg. These corr elations are dependent on the module’s channel length and ar e only valid for this specific module. Nonetheless, the principles for futur e module and pr ocess design remain equal for any geometry . For a given inlet feed concentration and a desired final concentration, R F must be determined in or der to achieve the r equir ed recovery ratio. Certain boundary conditions must also be considered. In or der to sustain overall e ffi ciency , the feed flow cannot be lower ed to a value that does not supply a su ffi cient amount of feed to MD 2. The negative e ff ects on GOR and thermal e ffi ciency were analyzed in Section 3.1 . In addition, a safety margin to pr event saturation of the solution in MD 2 should be added to the minimum feed flow rate. Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 22 of 30 Figure 15. Effe ct of H/C flow to feed flow rat i o R F on recovery ratio (RR); T hi ½ = 80 °C, T ci ½ = 25. The recommended proced ure for selection of feed inlet flow r a te and R F ca n be summa riz ed a s fol l ows: • Determ ina t io n of feed conc entr at ion; • Selec t ion of d e sire d outlet concentr ation ; • Selec t ion of r e qu ired R F; • Determ ina t io n of m i nimu m feed f l ow; • Calc ul at ion o f H / C f l ow r a te accord ing t o R F. Depending o n the available heat supply , the ch anne l leng th o f the module s w i ll be d e signed. Channel leng th se lect ion i s a key p a ram e ter in MD m o dule d e s i gn, both techno l o gic a l l y a s w e ll as economically as exp l ained in detail in [22]. Howeve r , the GOR and flux are muc h more sensitive to channel length modific atio n th an the ov eral l output o f the mo dule. In consequen c e, R F ra ti os ar e not expected to c h ange in a lar g e m a gnitude for the sa me t e mpera t ure p r ofi l e and cha nnel leng ths with in 4– 9 m . 3 . 4 . Comp arison with Sp iral Wound Air Gap Membrane Distillation (AGMD) Module W i t h i n t h i s w o r k s o f a r , a n o v e l t y p e o f M D con f ig uration w a s presented an d analy z ed. The ana l y s is wa s based upon a fir st -gen era t i o n proto t ype plate and frame module. A compar iso n with the previo usly stud ied spiral wo und A G MD module typ e shou ld nonethe l es s b e conduc ted at th is st age in o r d e r to id ent i f y an y pos s ib le d i s a dv an tage s of th e overall conc e p t. Even tho u gh the pack agin g of the modu les is di ff er ent , no signi fic a n t di ffe rence s in the inf l u e nce of oper at iona l parame ter s o n the K P Is o f the proce ss ar e expect e d. M a te rials and membrane ty pes are iden tical. The data use d for comparison is extr ac ted from a st u d y w i th an A G MD sp i r a l wound m o d u le and hypers a l i n e brine wh ic h can be fo un d wi th [ 4 9 ] . T h e AGMD m o dule h a d a 6 m ch anne l le ngt h and w a s oper ate d w i th the same flow o f 300 l/h. Error! Ref e r e nc e s o urce no t f o un d. sh ows flux and Fig u re 1 sho w s GOR v a l u es of bo th mo dule s in dir e c t compar ison . Flux va lue s f o r both mod u le t y pes are ve ry sim i l a r b u t wi th sl i g htl y h i gher val u es for the spir al woun d for t a p w a ter and sl igh t ly h i gher Figure 15. E ff ect of H / C flow to feed flow ratio R F on recovery ratio (RR); T hi 1 / 2 = 80 ◦ C, T ci 1 / 2 = 25. The r ecommended pr ocedure for selection of feed inlet flow rate and R F can be summarized as follows: • Determination of feed concentration; • Selection of desir ed outlet concentration; • Selection of r equir ed R F; • Determination of minimum feed flow; Membranes 2019 , 9 , 118 21 of 28 • Calculation of H / C flow rate accor ding to R F . Depending on the available heat supply , the channel length of the modules will be designed. Channel length selection is a key parameter in MD module design, both technologically as well as economically as explained in detail in [ 22 ]. However , the GOR and flux are much mor e sensitive to channel length modification than the overall output of the module. In consequence, R F ratios ar e not expected to change in a lar ge magnitude for the same temperatur e pr ofile and channel lengths within 4–9 m. 3.4. Comparison with Spiral W ound Air Gap Membrane Distillation (AGMD) Module W ithin this work so far , a novel type of MD configuration was pr esented and analyzed. The analysis was based upon a first-generation pr ototype plate and frame module. A comparison with the previously studied spiral wound AGMD module type should nonetheless be conducted at this stage in or der to identify any possible disadvantages of the overall concept. Even though the packaging of the modules is di ff er ent, no significant di ff erences in the influence of operational parameters on the KPIs of the pr ocess ar e expected. Materials and membrane types ar e identical. The data used for comparison is extracted fr om a study with an AGMD spiral wound module and hypersaline brine which can be found with [ 49 ]. The AGMD module had a 6 m channel length and was operated with the same flow of 300 L / h. Figure 16 shows flux and Figur e 17 shows GOR values of both modules in direct comparison. Flux values for both module types are very similar but with slightly higher values for the spiral wound for tap water and slightly higher values for the plate and frame for at salinities above ~80 g NaCl / kg. This shows that for a similar channel length and under the same operating conditions r egarding the heating and cooling flows, the flux is similar r egar dless of the module type. The internal heat recovery of the modules expr essed as GOR, however , shows some di ff er ences especially at tap water salinity . This e ff ect can be assigned to the additional heat-transfer r esistance added by the feed gap in the plate and frame. In the low-salinity region wher e vapour pr essur e depreciation does not have an impact, the lar ger delta T caused by the additional thermal r esistance leads to a higher ener gy r equir ement per mass unit of distillate which dir ectly e ff ects the GOR. At the same time, this higher e ff ective delta T leads to advantages over the spiral wound module at higher conductivities since mor e net driving for ce is available after subtracting the fraction of driving for ce lost to the r eduction in vapour pr essure. The asymmetrical temperature pr ofiles in the FGAGMD module shown in Section 3.1 . also account for a reduction in the overall GOR values of this module type. When c ompa ring r ecovery r atio a nd the rmal effi cien cy sho wn in Fi gure 1 8 , the most s igni ficant diff er ence is i n the r ecov ery ra tio. At tap wate r the d iffe r ence is 70% and at 214 g Na Cl / k g the diffe r ence is sti ll app rox imat ely 30 %. The ena blin g of such hig h r ecovery r atios was o ne of th e cor e motiv ations fo r the im plem entatio n of the n ew FGAGMD c hann el config urat ion. As menti oned pr evious ly , the r ecovery rati o of the s piral wou nd AGM D module is n ot ind ependen tly ad justabl e due to t he cou pling of he at supp ly and feed s upply . Ther mal ef ficienc y valu es ar e simi lar fo r both modu les wi th the lar gest diff er ences a t the lo w end of t he sal init y rang e. On averag e for the ent ir e salini ty range te sted , howe ver , η th of t he FGA GMD mo dule was hi gher b y appr oximate ly 4% compa r ed to the spi ral wound m odule. Fr om the dir ect comparison of the two module types, it can be deducted that even in this first pr ototype stage, the plate and frame (PF) FGAGMD module has a general advantage over the spiral wound (SW) AGMD module when implemented in high concentration applications. Under the assumption that e.g., a RO brine at a salinity 7 g NaCl / kg should be concentrated to 240 g NaCl / kg [ 22 ], at the r esulting avg. salinity of 155 g NaCl / kg the FGAGMD module is be superior in performance r egar ding flux, η th and RR with only small drawbacks in GOR. T able 4 pr ovides a summary of KPIs at the mentioned avg. salinity of 155 g NaCl / kg. Membranes 2019 , 9 , 118 22 of 28 Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 23 of 30 values for th e plate and fr ame for at salinities above ∼ 80 g NaC l /kg. This sho w s th at for a similar channel leng t h and und e r the s a me ope r at ing cond i t i o ns reg a rd in g the he a t ing and cool ing flows , the f l ux i s sim i l a r reg a rd les s o f the m o d u le typ e . T h e i n tern al he at r e cov e ry o f th e m o d u le s ex p r essed as GO R, how e ver, shows some differenc e s espec i ally at t a p wa ter s a l i ni ty. This e ffec t c a n be a s signe d to the ad di tio n al he at -t ran s fer res i s t ance ad ded b y th e fe ed gap in the plate an d fr ame. In the low - salin ity reg i o n where vapo ur pressure d epreciation d o es not h a ve an impact, th e larger delta T caused b y th e add i ti onal therm a l resi st ance le a d s to a h i gh er ener gy re quirement per mass unit o f distillate which d i rec t l y ef fec t s the GOR. At th e same t i me, th is h i gher e ffe ctive de lt a T lea d s to adv a nta ges ove r t h e s p i r al wou n d modu l e a t hi g h e r c o nd u c ti vit i e s since more net driv ing fo rce is ava i l a bl e af ter subtr a c t in g t h e fr ac tion of driv ing forc e lo st to the re duct ion in va pour pre s s u r e . The a s ym metric a l temper ature profiles in th e FGAGMD module show n in Sect ion 3 . 1. a l so acco u n t fo r a red u c t ion in the over all G O R v a lues o f this module type. When comp a ring recovery ra t i o and the rmal ef fic ie nc y shown in F i gure 2, the m o st signific an t difference is in the recove ry r a tio. A t tap w a t e r the di ffe rence i s 7 0 % and at 21 4 g N a C l /k g the dif f erence is s t i ll approxim ate l y 3 0 %. Th e enabling o f such h i gh rec o very ratios was one of th e core motiv a t i ons f o r the impl e m enta ti on of the new FG AGMD ch an nel con fig ur a t ion. A s men t ione d previously , the recovery r a tio of the sp iral woun d A G MD module is no t inde pendently ad justable due to the co uplin g o f h e at supply and feed supply. The r ma l ef fi ci e n c y val u es a r e si mi la r f o r bot h module s w i th the lar g est difference s at the low en d of t h e sa li nity ra ng e. On ave r a g e f o r t h e e n t i r e sa lin ity r a ng e tes t ed, ho wever, η th of th e FG AG MD m o d u le was hi gher b y ap p r ox im ate l y 4% compared to the spir al wo und mod u le . From the d i r e ct com p ar is on of the two m o dule typ e s, i t can b e d e d uct ed th a t e v en in th is f i r s t prototype stage, the p l ate and fr ame (PF ) FGAGMD m o dule has a g e neral advan t age ov er the spiral wound (SW ) AGMD mo dule when implemented in high conc entration ap plic at ions. U n der the ass u m p t i on t h at e.g ., a RO b r ine a t a s a l i ni ty 7 g N a C l /k g sho u l d b e concent r a t e d to 2 4 0 g N a C l /k g [2 2] , a t the r e su lt ing avg . s a l i ni ty of 15 5 g N a Cl / kg the FGA G MD modu l e i s be s u pe rior in performanc e regar d ing flux, η th and R R with onl y sm al l drawb a ck s in G O R. Err o r! Refer e nc e sourc e not f ound . p r ovides a sum m ary o f K P Is at the m e nt io ned av g. sa lin ity of 1 5 5 g N a C l /kg . Figure 16. Infl u e nce of conce n trate salini ty on flu x in plat e and frame F G AGMD and spiral wound AGMD mod u les ; 𝒗 𝒇 = 40 kg/h, 𝒗 𝑯/ 𝑪 = 300 l/ h per module; 𝒗 𝒇𝒔𝒘 = 300 l/h; T hi = 80 °C, T ci = 2 5 Figure 16. Influence of concentrate salinity on flux in plate and frame FGAGMD and spiral wound AGMD modules; . v f = 40 kg / h, . v H / C = 300 L / h per module; . v f sw = 300 L / h; T hi = 80 ◦ C, T ci = 25. Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 24 of 30 Figure 1 . Influ e nce of concen trate salin ity o n GOR in plat e and frame FGAGMD and spiral wound AGMD mod u les ; 𝒗 𝒇 = 40 kg/h, 𝒗 𝑯/ 𝑪 = 300 l/ h per module; 𝒗 𝒇𝒔𝒘 = 300 l/h; T hi = 80 °C, T ci = 25 Figure 2. Influ e nce of con c entrate sal i nity o n thermal effi ci ency η th and re covery ratio (R R) in plat e and frame and spiral wou n d modu le typ e s u n der simil a r operating co nditions ; 𝒗 𝒇 = 40 kg/h, 𝒗 𝑯/𝑪 = 300 l/ h per mo dule; 𝒗 𝒇𝒔𝒘 = 300 l/h; T hi = 80 °C, T ci = 25 Fur t her po te ntial fo r improvement on the plate and frame modu l e des ign i s d e fin ite l y g i ve n, especially re g a rd ing flow d i stribution an d channe l ge ometry . It is e x pected that similar GOR values Figure 17. Influence of concentrate salinity on GOR in plate and frame FGAGMD and spiral wound AGMD modules; . v f = 40 kg / h, . v H / C = 300 L / h per module; . v f sw = 300 L / h; T hi = 80 ◦ C, T ci = 25. Membranes 2019 , 9 , 118 23 of 28 Mem b ranes 2019 , 9 , x FO R P EER R E VIEW 24 of 30 Figure 1 . Influ e nce of concen trate salin ity o n GOR in plat e and frame FGAGMD and spiral wound AGMD mod u les ; 𝒗 𝒇 = 40 kg/h, 𝒗 𝑯/ 𝑪 = 300 l/ h per module; 𝒗 𝒇𝒔𝒘 = 300 l/h; T hi = 80 °C, T ci = 25 Figure 2. Influ e nce of con c entrate sal i nity o n thermal effi ci ency η th and re covery ratio (R R) in plat e and frame and spiral wou n d modu le typ e s u n der simil a r operating co nditions ; 𝒗 𝒇 = 40 kg/h, 𝒗 𝑯/𝑪 = 300 l/ h per mo dule; 𝒗 𝒇𝒔𝒘 = 300 l/h; T hi = 80 °C, T ci = 25 Fur t her po te ntial fo r improvement on the plate and frame modu l e des ign i s d e fin ite l y g i ve n, especially re g a rd ing flow d i stribution an d channe l ge ometry . It is e x pected that similar GOR values Figure 18. Influence of concentrate salinity on thermal e ffi ciency η th and r ecovery ratio (RR) in plate and frame and spiral wound module types under similar operating conditions; . v f = 40 kg / h, . v H / C = 300 L / h per module; . v f sw = 300 L / h; T hi = 80 ◦ C, T ci = 25. Further potential for impr ovement on the plate and frame module design is definitely given, especially r egar ding flow distribution and channel geometry . It is expected that similar GOR values to the AGMD module will be possible after optimization of the inner components of the module. Furthermor e, an incr ease in channel length can be consider ed in order to incr ease the GOR. This will, however , decrease the flux and r equire mor e membrane area. The application of vacuum to the air gap would have a significant positive e ff ect on e ffi ciency , though drawbacks in distillate quality are to be expected when implementing this option. T able 4. A verage key performance indicator (KPI) values for plate and frame FGAGMD and spiral wound AGMD module, mean concentrate salinity ~155 mS / cm; . v f = 40 kg / h, . v H / C = 300 L / h per module; . v f sw = 300 L / h; T hi = 80 ◦ C, T ci = 25. Flux GOR RR η th (kg / m 2 h) (-) (%) (%) PF FGAGMD 1.2 1.1 45 50 SW AGMD 1.1 1.4 3 46 4. Conclusions W ithin this work, a novel plate and frame FGAGMD module was pr esented. By separating the heating and cooling channel from the feed channel, the concept allows a minimum amount of components in contact with the highly corr osive feed. Furthermor e, it decoupled the thermal ener gy supply fr om the feed supply , giving room for a new range of operational flow settings. The goal of incr easing the recovery ratio of the single pass pr ocess was achieved with values of up to 93% RR using tap water as feed and between 32–53% with NaCl solutions ranging between 117 and 214 g NaCl / kg. The impact of well-known corr elations on the KPIs flux, GOR and η th r emained valid for this new module type. For optimization of flow rate strategies for a given range of concentration a new ratio of H / C flow to feed flow was introduced named R F . R F serves as an indicator for the Membranes 2019 , 9 , 118 24 of 28 selection of a flow r egime to achieve a r equired r ecovery ratio. In comparison to a previously analyzed AGMD spiral wound module, the FGAGMD plate and frame pr ototype showed similar performance characteristics with slight impr ovements r egarding flux and η th . As expected, the recovery ratio was between 12–16 times higher in the plate and frame module (32–93%) than in the spiral wound (2–6%) due to the new channel configuration. Drawbacks of the FGAGMD module were observed in GOR especially in the lower salinity r egion. For an average salinity of 155 mS / cm, however , the di ff erence in GOR r educed approx. 0.3. It is likely that the GOR of the plate and frame module can be improved by optimizing the internal flow distribution within the channels which was not the focus in the construction of this first pr ototype module. In general, for the applications with corrosive, toxic or otherwise hazar dous media the implementation of a FGAGMD plate and frame MD module opens up a new range of applications for the technology with advantages in cleaning and maintenance, safety and the integration into industrial wastewater tr eatment processes. Further impr ovements must be carried out to optimize the e ffi ciency and long- term testing will be necessary with a follow-up pr ototype in or der to properly evaluate lifetime cycles of all r eplacement parts. Furthermor e, an in depth investigation of the thermodynamics of the FGAGMD process in a flat sheet bench scale testing facility will published in a follow-up publication. This will enable the validation of modelling tools and the optimization of e ffi ciency and operational key factor R F with r espect to di ff er ent salinity levels. Author Contributions: R.S. was the lead investigator and author of the original manuscript. She pr ovided the methodology , and final data evaluation and managed and supervised the pilot operation. The prototype module was conceptualized by R.S. and L.B. L.B. constructed and built the pr ototype. J.S. operated the prototype, conducted preliminary data evaluation and was supervised by R.S. and T .H. Expert input regar ding the methodology , and draft review was pr ovided by D.W . and J.K. Further reviewing and editing was conducted by T .H. and S.-U.G. Funding: This resear ch was funded by the German Federal Ministry of Education and Research, grant number 02W A V1406E. Conflicts of Interest: The authors declare no conflict of inter est. The founding sponsors had no role in the design of the study; in the collection, analyses, or interpretation of data; in the writing of the manuscript; and in the decision to publish the results. Nomenclature A Membrane area AGMD Air gap membrane distillation C Conductivity (mS / cm; µ S / cm) cp Specific heat capacity (kJ / kg K) DCMD Direct contact membrane distillation delta T Driving force temperatur e di ff erence (K) dTh T emperature di ff er ence on the hot side of the module dT c T emperature di ff er ence on the cold side of the module F Flow (L / h) FGMD Feed Gap Membrane Distillation FGAGMD Feed Gap Air Gap Membrane Distillation GOR Gained output ratio ( - ) h Height (m) HEX Heat exchanger KPI Key performance indicator m Mass flow (kg / h) MD Membrane Distillation MED Multi E ff ect Distillation MSF Multi Stage Flash j T ransmembrane flux (kg / m 2 h) L Channel length (m) p Pressur e (bar) P Pump Membranes 2019 , 9 , 118 25 of 28 PP Polypropylene PTFE Polytetrafluorethylene PGMD Permeate gap membrane distillation R Ratio RR Recovery ratio RO Reverse Osmosis S Salinity (g / kg) SWRO Seawater Reverse Osmosis T T emperature ( ◦ C) ρ Density (kg / m 3 ] η E ffi ciency (%) v-AGMD V acuum air gap membrane distillation v V olume flow (L / h) ∆ hv Evaporation enthalpy (kJ / kg) Indices ci cooling inlet co cooling outlet d distillate hi heating inlet ho heating outlet f feed F feed ratio H / C heating and cooling hx heat exchanger m mean th thermal References 1. 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