Jou nal o Wa e P ocess Enginee ing 46 (2022) 102587
A ailable online 3 Feb ua y 2022
2214-7144/© 2022 The Au ho s. Published by Else ie L d. This is an open access a icle unde he CC BY license (h p://c ea i ecommons.o g/licenses/by/4.0/).
Benchma king e ia y wa e ea men s o he emo al o mic opollu an s
and pa hogens based on ope a ional and sus ainabili y c i e ia
Sab ina de Boe
1
, Jo ge Gonz´
alez-Rod íguez
*
,
1
, Julio J. Conde
1
, Ma ia Te esa Mo ei a
a
CRETUS, Depa men o Chemical Enginee ing, Uni e sidade de San iago de Compos ela, 15782 San iago de Compos ela, Galicia, Spain
ARTICLE INFO
Keywo ds:
Re iew
Te ia y ea men
LCA
Economic e alua ion
Eme ging pollu an s
ABSTRACT
In a con ex o inc easing wa e sca ci y, i is essen ial o ensu e an in eg a ed wa e shed managemen , sa ings in
he consump ion o wa e as a ini e esou ce and imp o e he pe o mance o was ewa e ea men plan s o
gua an ee he quali y o ea ed e luen s. The e o e, ad anced echnologies o e ia y was ewa e ea men
ha e been widely s udied in ecen decades. These ea men s ha e been e iewed o e he yea s mainly
p o iding compa isons om a echnical pe spec i e. Howe e , he e is a lack o a holis ic e alua ion conside ing
en i onmen al and economic aspec s oge he wi h he a o emen ioned echnical aspec s. In his e iew, ea -
men al e na i es o mic opollu an and pa hogen aba emen ha e been iden i ied based on echnologies
implemen ed on a la ge scale (ozona ion, ul a iole ea men , adso p ion on ac i a ed ca bon o memb ane
il a ion) as well as hose ea men s in he p ocess o implemen a ion, such as elec ochemical, Fen on-based o
pho oca aly ic echniques. Thus, a sys ema ic bibliog aphic sea ch was pe o med conside ing wo ks applying
pilo and ull-scale equipmen , lea ing lab-scale esul s ou o he analysis. The desc ip ion o each p ocess
allowed he iden i ica ion o he echnical easibili y, ope a ing cos s and associa ed en i onmen al impac s,
p o iding a compa a i e assessmen ha will help decision-making in he de elopmen and applica ion o he
di e en echnologies. The benchma king esul s e eal ha he selec ed ea men should be chosen based on
he sou ce and speci ic pollu an s p esen in he was ewa e , as he e is no single solu ion o he ea men o
mic opollu an s and pa hogens. In addi ion, ecommenda ions a e p esen ed o he publica ion o eliable
p ocess- ela ed da a o acili a e compa ison be ween di e en echnologies and ea men scena ios.
1. In oduc ion
Popula ion g ow h implies an inc easing demand o na u al e-
sou ces such as wa e , ene gy and ood [1]. In his con ex , one o he
mos se ious p oblems o be aced is he inc easing wa e sca ci y [2].
This concep is de ined as he imbalance be ween wa e demand and
a ailabili y and is ela ed o unbalanced consump ion o wa e ese es,
declining quali y o d inking wa e due o con amina ion o saline
in usion o su ace wa e s and aqui e s and inc eased pe iods o
d ough [3]. The impo ance o access o sa e d inking wa e and sani-
a ion is highligh ed and embedded in Goal 6 o he Uni ed Na ions
Sus ainable De elopmen Goals [4]. In o de o add ess he p oblems
ela ed o wa e pollu ion, la ge in es men s ha e been made in
was ewa e ea men plan s (WWTPs) [5]. Al hough WWTPs a e
capable o emo ing o ganic ma e and nu ien s (ni ogen and phos-
pho ous), he occu ence o o ganic mic opollu an s (OMPs) such as
pe sonal ca e p oduc s, pes icides, endoc ine dis up ing chemicals o
pha maceu icals, in di e en en i onmen al compa men s equi es
changes in he design and ope a ion o was ewa e acili ies o ensu e
hei emo al and he quali y o he ea ed e luen s [6,7].
As pa o he implemen a ion o he Wa e F amewo k Di ec i e, he
Eu opean Union de ined a lis o p io i y subs ances ha could pose a
isk o he en i onmen and human heal h. The “Wa ch Lis ” epo ed in
2015 included wo pha maceu icals, na u al ho mones, h ee mac olide
an ibio ics, pes icides, an ul a iole il e and an an ioxidan . Subse-
quen ly, h ee addi ional subs ances we e added in 2018: an insec icide
and wo an ibio ics. Wi h he p ima y objec i e o OMPs emo al, some
e ia y ea men echnologies, such as memb ane il a ion o
adso p ion on ac i a ed ca bon, allow he e en ion o OMPs om he
was ewa e s eam. Howe e , he concen a ed low and he spen
adso ben ha e o be con enien ly managed in a downs eam p ocess
inc easing he complexi y o hese echniques [8]. The possibili y o
* Co esponding au ho .
E-mail add ess: [email p o ec ed] (J. Gonz´
alez-Rod íguez).
1
Sab ina de Boe , Jo ge Gonz´
alez-Rod íguez and Julio J. Conde ha e con ibu ed o he manusc ip equally.
Con en s lis s a ailable a ScienceDi ec
Jou nal o Wa e P ocess Enginee ing
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h ps://doi.o g/10.1016/j.jwpe.2022.102587
Recei ed 3 Oc obe 2021; Recei ed in e ised o m 30 No embe 2021; Accep ed 16 Janua y 2022
Jou nal o Wa e P ocess Enginee ing 46 (2022) 102587
2
implemen ing ad anced oxida ion p ocesses (AOPs) based on non-
speci ic oxida ion mechanisms [9] such as ozona ion o UV adia ion
a e op ions ha ha e had a iable success since hei la ge-scale ope -
a ion in ol es high ope a ing cos s due o hei high ene gy e-
qui emen s o lowe kine ic a es.
Beyond o ganic mic opollu an s, special a en ion should be also
paid o con amina ion by hea y me als, which a e gene ally classi ied as
ino ganic mic opollu an as hey a e p esen in ea ed e luen s in ace
concen a ions. Con amina ion due o hea y me als can occu na u ally,
caused by he en ainmen o geological ma e ial in o su ace wa e s
al hough mos hea y me al pollu ion has been de e mined o be
an h opogenic, de i ing om he use o pes icides and ungicides (As) o
pigmen s (As, Cd, C , Cu, Pb, Ni), as well as om he me allu gical (As,
Cd, Hg), pe ochemical (Cd, Pb) o py o echnical (As) sec o s [10]. In
his e iew, pa hogen emo al is also conside ed o benchma king since
e ia y ea men s a e widely used as me hods o pa hogen aba emen
[11]. The p esence o pa hogens is especially ele an in u ban, hospi al,
li es ock and ag icul u al was ewa e , since he elease o mic oo gan-
isms in o wa e bodies con ibu es o he sp ead o pa hogens and
an ibio ic esis ances.
Se e al e iew a icles ha e ecen ly been published on he bene i s
and d awbacks o ad anced e ia y ea men s o was ewa e polish-
ing, mainly ocusing on he echnological aspec s o ea men s. Fo
ins ance, expe s om NEREUS COST Ac ion analyzed he bes a ailable
echnologies o wa e euse o c op i iga ion conside ing ozona ion,
ac i a ed ca bon adso p ion, chemical disin ec an s, UV adia ion,
ad anced oxida ion p ocesses and memb ane il a ion [12]. The
conclusion o he expe g oup is ha a single ad anced ea men
me hod is no su icien o minimize he elease o chemicals o
eme ging conce n and an ibio ic- esis an mic oo ganisms. Luo e al.
analyzed he emo al e iciency o he selec ed mic opollu an s in 14
coun ies and egions, analyzing di e en e ia y sys ems such as
coagula ion– loccula ion, ac i a ed ca bon adso p ion, ad anced
oxida ion p ocesses, nano il a ion, e e se osmosis, and memb ane
bio eac o s [13]. Rizzo e al. analyzed consolida ed e sus new e ia y
ea men me hods, concluding ha he lack o compa a i e esea ch
be ween he wo ca ego ies complica es he e alua ion o he mos
sui able and cos -e ec i e solu ion o he ea men o eme ging con-
aminan s [14]. Bui e al. pe o med a mul ic i e ia assessmen o
ad anced ea men echnologies o mic opollu an s emo al,
including e y b ie e e ences o en i onmen al conside a ions and
only including some o he a ailable e ia y ea men s, i.e., adso p ion,
ozona ion, UV/H
2
O
2
, memb ane p ocesses and memb ane bio eac o s
[15].
The analyzed e iews a e mainly ocused on he echnical aspec s,
lacking he economic and en i onmen al pe spec i es. The sea ch o
new echnological al e na i es mus mee he ollowing objec i es:
echnological easibili y in he cons uc ion and ope a ion o he
equipmen , ope a ional e iciency and eliabili y and educ ion o
en i onmen al impac s and cos s. Based on he sco e in each o he
a o emen ioned sec ions, decision making will be be e suppo ed by
e idence and con as able da a [16]. In acco dance wi h Eu opean di-
ec i es, en i onmen al and socioeconomic ac o s, including consid-
e a ion o human heal h, mus be conside ed in he assessmen o
ad anced echnologies. In his sense, he en i onmen al impac s asso-
cia ed wi h e ia y ea men s can be elucida ed using he in e na-
ionally s anda dized Li e Cycle Assessmen (LCA) me hodology.
Conside ing he en i onmen al app oach, Pesquei a e al. conduc ed a
li e a u e e iew solely on he applica ion o LCA in e ia y was ewa e
ea men , howe e , he scope o he e iew ocuses on he emo al o
p io i y subs ances and pollu an s o eme ging conce n men ioned in
Eu opean legisla ion, including a o al o 18 pape s [17]. In his s udy,
he ocus was u he ex ended o a o al o 40 pape s dealing wi h LCA
in e ia y ea men s.
In consequence, he main objec i e o his keywo d-based li e a u e
e iew is o pe o m a holis ic analysis o he main echnological
de elopmen s in e ia y ea men s om a sus ainabili y pe spec i e,
including no only e iciency a iables, bu also en i onmen al impac s
and cos es ima ion. The key aspec s o he echnologies we e iden i ied
and e alua ed o pilo and ull-scale s udies conside ing echnical and
sus ainabili y app oaches, concluding ha he combina ion o mul iple
ea men p ocesses is essen ial o mee he e luen equi emen s.
Mo eo e , he use o LCA me hodology as a powe ul ool o decision-
making can highligh speci ic ho spo s o he echnologies, com-
plemen ing he in o ma ion p o ided by economical and echnological
e alua ion. Acco dingly, he main challenge is o emphasize he key da a
o each echnology conside ing a join echnical, en i onmen al, and
economic app oach, p o iding use ul in o ma ion abou he main
d awbacks o p esen s udies and desi able a ge s o u u e esea ch.
2. Bibliog aphic sea ch me hodology
The li e a u e sea ch was pe o med using he sea ch ool p o ided
by he SCOPUS da abase in Ma ch 2021. The selec ion o manusc ip s
add essing he e iciency o e ia y was ewa e ea men s o he
emo al o mic opollu an s unde echnological, economic and en i-
onmen al c i e ia was conduc ed. Conside ing he scope o he e iew,
he sea ch was limi ed o he echnologies applied o was ewa e ea -
men , including he keywo ds “was ewa e ea men ” o “was e wa e
ea men ” in he sea ch s ing. In addi ion, since he goal o e ia y
ea men s is he emo al o mic opollu an s, hea y me als and pa ho-
gens, hese wo ds and hei ele an abb e ia ions we e conside ed in
he o mula ion o sea ch pa ame e s by including hei espec i e
keywo ds. Fo his pu pose, he sea ch p ocedu e used in he li e a u e
e iew is summa ized in Fig. 1, along wi h he speci ic keywo ds and
Boolean ope a o s.
Te ia y ea men s we e classi ied in o se en dis inc g oups o
acili a e he sea ch p ocess, i.e., ozona ion, ul a iole , ca alys -based,
p essu e-d i en, ac i a ed ca bon adso p ion, elec ochemical and
i adia ion ea men s. Mo eo e , he esul s we e il e ed and educed
conside ing hei publica ion a e 2010, w i en in English and in a inal
s ep o publica ion. The ob ained esul s applying each s ep a e p e-
sen ed in he Table S1 in he Elec onic Suppo Ma e ial (ESM) 1. The
analysis o en i onmen al indica o s es ima ed by he LCA me hodology
ha e been also analyzed pe o ming a complemen a y sea ch, using
speci ic keywo ds as “li e cycle” o “LCA”.
The esul s o he bibliog aphic sea ch a e compiled in ESM 2 and
ESM 3 in he Supplemen a y In o ma ion. ESM 2 includes he biblio-
g aphic in o ma ion o all s udies analyzed a e he second e ining s ep
along wi h hei basic bibliog aphic da a, while ESM 3 p esen s a s an-
da dized able wi h he echnoeconomic da a ex ac ed om he
selec ed s udies, ocusing in mic opollu an emo al and ope a ional
condi ions.
3. Bibliome ic analysis
The bibliome ic analysis includes all he esul s a e he manual
e inemen ob ained om Scopus using he me hodology explained
abo e. These pape s ha e been aken in o accoun o he echnological
and economic analysis pe o med du ing his e iew, and he keywo ds
we e ex ac ed and analyzed acco ding o hei occu ence and e-
la ionships, as shown in Fig. 2. To cla i y he da a and homogenize he
esul s, he subs i u ion o keywo ds by synonyms o abb e ia ions was
conduc ed conside ing he o ma ion o clus e s in ol ing keywo ds
wi h high simila i y (ESM 4).
In iew o he esul s, he keywo ds can be classi ied in o ou g oups
conside ing he main opic add essed: (i) gene ic keywo ds: his g oup
o med by was ewa e ea men , e ia y ea men s, was ewa e euse
and domes ic was ewa e , e ms ha ep esen he a ge o he indings
and he de ini ion o he ield o s udy; (ii) a ge compound: he mos
epea ed keywo ds we e pha maceu icals and pe sonal ca e p oduc s
(PPCPs), o ganic mic opollu an s (OMPs), compounds o eme ging
S. de Boe e al.
Jou nal o Wa e P ocess Enginee ing 46 (2022) 102587
3
Fig. 1. Sea ch me hodology o he di e en e ia y ea men s.
Fig. 2. Map and ne wo k o keywo ds (elabo a ed wi h VosViewe ®).
S. de Boe e al.
Jou nal o Wa e P ocess Enginee ing 46 (2022) 102587
4
conce n (CECs) and an ibio ics (ABs) and ep esen he main a ge
compounds e alua ed; (iii) echnologies: his g oup encompasses he
di e en echnologies used o e ia y was ewa e ea men such as
il a ion, ozona ion, UV o AOPs; and (i ) ea men e ec i eness: his
g oup includes he me hods ca ied ou o he e alua ion o he ech-
nologies, such as emo al, emo al e iciency, by-p oduc s iden i ica ion
o oxici y.
Fig. 2 allows e ia y ea men s o be classi ied be ween la ge-scale
applied echnologies and mo e inno a i e p ocesses, and hese ends
a e ep esen ed in he diag am. Focusing on he was ewa e ea men
ci cle and i s ela ionships, his keywo d usually appea s oge he wi h
adso p ion echniques as g anula ed ac i a ed ca bon o powde ed
ac i a ed ca bon (GAC-PAC), ozona ion, il a ion and UV, indica ing
ha he echnologies mos applied as ad anced ea men s o he
emo al o PPCPs and OMPs a e hose men ioned abo e.
On he o he hand, he e is an e iden ela ionship be ween e ia y
ea men and i ania, pho oca alysis and sola ea men , as well as a
g owing in e es in pa hogen emo al. This keywo d appea s ela ed o
o he s such as disin ec ion o p esence in wa e o an ibio ic esis an
bac e ia (ARBs) and an ibio ic esis ance genes (ARGs), showing he
cu en conce ns ega ding he ans e o an ibio ic esis ance o pa h-
ogens in he en i onmen . Ano he issue o highligh is he close ela-
ionship be ween elec ochemical me hods and hea y me als (HMs),
showing he p e e ences o he use o his ype o p ocesses o he
ea men o was ewa e con aining hea y me als. Adso p ion ech-
niques such as GAC-PAC and il a ion-based ea men s o emo e
con aminan s we e usually s udied oge he , as can be seen by he
p oximi y o poin s and wid h o he ela ion line. In gene al, low
p esence o c oss-sec ional keywo ds as “economic assessmen ” was
obse ed conside ing he signi icance c i e ia (only wo ds wi h an
occu ence o mo e han 3 we e conside ed o he s udy). As a esul ,
al hough some a icles inco po a e he economic e alua ion o he
echnology, he analysis om he en i onmen al poin o iew is
missing.
4. Technological aspec s o e ia y ea men s
4.1. Ozone-based ea men s
Ozona ion (O₃₃) is a he e ogeneous p ocess applied o he oxida i e
Fig. 3. A) Schema ic ep esen a ion o an ozone ea men uni . B) Wo ldwide dis ibu ion o he analyzed s udies (ci cle a ea is p opo ional o he ea ed low a e
and colo ep esen he con inen ). C) O e iew o he quali y equi emen s o he in luen and ypical ope a ional pa ame e s and consumables anges o he
analyzed s udies. D) Remo al e iciencies o he mos in es iga ed compounds (n >2). The ac onym lis is a ailable in Supplemen a y In o ma ion (ESM 3).
S. de Boe e al.
Jou nal o Wa e P ocess Enginee ing 46 (2022) 102587
5
ea men o d inking wa e and mo e ecen ly o was ewa e .
Con e sely o ully wa e miscible oxidan s (e.g., H₂O₂), mass ans e
op imiza ion om he gaseous o he aqueous phase mus be conside ed.
Typically, bubble column eac o s a e used o con ac he ozone wi h he
wa e s eam (Fig. 3A). Ozona ion has been s udied mainly in con in-
uous p ocesses, whe eas ba ch ope a ion is he se up o choice a pilo
scale o op imize eac ion condi ions [18–20]. Mos o he e iewed
s udies conside ed he applica ion o ozona ion o e luen s om con-
en ional seconda y ea men plan s. Howe e , since ozona ion uses
non-speci ic oxida ion pa hways o ans o m a ge compounds, he
e sa ili y o his p ocess allows i s wide applica ion, such as o he
emo al o pollu an s om su ace g oundwa e s [21–23] as well as
o he ypes o was ewa e s, e.g., indus ial e luen s [24,25] o ejec
s eams om ul a il a ion and e e se osmosis uni s [26]. 70% o he
e iewed s udies we e loca ed in Eu ope, whe eas none o hem was in
A ica, as depic ed in Fig. 3C.
The ypical empe a u e o ozona ion- ea ed e luen s anges om
10 o 30 ◦C depending on clima ic condi ions and WWTP loca ion, high
empe a u es can lead o ola iliza ion o compounds acili a ed by gas
bubbling. In gene al, a pH abo e 8 a o s ozone decomposi ion medi-
a ed by hyd oxyl anions, bu his condi ion is no me in mos was e-
wa e s, he pH alues in he selec ed s udies a y in he ange o 6.0 o
10.5, espec i ely. To a much g ea e ex en han hyd oxyl anions, dis-
sol ed o ganic ma e (e.g., phenols and amines) induces he o ma ion
o hyd oxyl adicals h ough di e en pa hways [27,28]. I should be
no ed ha he e iciency o he p ocess can be hampe ed by high load-
ings o adical sca enging species such as ca bona es, halogen ions o
ni ogen oxides [29,30]. Consequen ly, he abundance o hese species
implies no only a educ ion o he ea men e iciency bu also he
o ma ion o oxic oxida ion p oduc s when halogen ions a e p esen in
he eac ion ma ix (b oma e o ma ion). In a ypical con igu a ion,
ela i ely sho emo al imes o achie e mic opollu an emo al a y
om 5 o 30 min, bu can ex end o longe pe iods, as is he case o
nonylphenol o bisphenol-A wi h ea men imes up o 100 min [31]. In
he case o o ganic ma e emo al, i has been es ablished ha he
ozone dose a ies depending on he s eam low o be ea ed be ween
alues o 1 o 200 mg O₃ L
−1
.The ypical pa ame e s o ozona ion a e
p esen ed in Fig. 3B.
The elec ophilic cha ac e o ozone and i s high oxida ion po en ial
(E
0
=2.07 V) enhance i s eac i i y owa ds compounds wi h low
oxida ion s a e such as dep o ona ed amines, sul ides, and a oma ic
ings wi h elec on dono g oups [29,32,33]. In addi ion o di ec
oxida ion, he e a e indi ec oxida ion pa hways in which eac i e ox-
ygen species (ROS), mos no ably •OH adicals, a e p oduced [29,30],
leading o he decomposi ion o wa e pollu an s due o hei high
oxida ion po en ial (E
0
=2.80 V), as seen in Fig. 3D [34]. The s udied
pollu an concen a ions a e in he ange o 0.1 ng L
−1
and 1.5 mg L
−1
o pha maceu icals and pes icides, and om 1 mg L
−1
o 500 mg L
−1
o
he combina ion o ozona ion wi h an elec ochemical me hod [25].
Al hough mos au ho s ocus hei esea ch on ozone-media ed mic o-
pollu an emo al, some wo ks ha e s udied deg ada ion pa hways as
well as he consequences o ea men on he ea ed e luen in e ms o
oxici y, es ogenici y o mu agenici y [31,35,36]. Di e en species
ha e been conside ed o in i o s udies on he po en ial mu agenici y
and oxici y o he ea men , in pa icula using Daphnia magna [37],
Alii ib io ische i [37,38] and Po amopy gus an ipoda um [39]. Fu he -
mo e, he o ma ion o in e media es [40] o he in luence o ozona ion
on ARGs and ARBs [38,41] ha e been s udied. As a special case, he
applica ion o his p ocess alone o in combina ion wi h GAC and sand
il e agains inac i a ion o mic oo ganisms p o ided educ ions o up
o 4.3 log emo al alue (LRV) o En e ococci and Esche ichia coli bac-
e ia [41–43]. Unlike in chlo ina ion, he o ma ion o by-p oduc s
a ec ing wa e quali y such as haloalkanes is p e en ed [44].
To imp o e i s e iciency and pollu an emo al pe o mance,
ozona ion can be combined wi h UV i adia ion [23,45] and hyd ogen
pe oxide [26,37]. UV ligh a wa eleng hs up o 310 nm p o okes he
dissocia ion o O
3
in o an oxygen molecule and hyd ogen pe oxide.
Simila ly, he pe oxone p ocess (O₃₃-H₂₂O₂₂) combines he oxidizing
powe o ozone wi h he decomposi ion o H₂O₂ o enhance he gene -
a ion o •OH adicals and has been shown o be e ec i e in educing
ozone- esis an mic opollu an s [27]. One o he mos impo an ac o s
o conside in he pe oxone p ocess is he a io o O₃ o H₂O₂, which
go e ns he eac ion a e. Howe e , he high capaci y o H
2
O
2
ega ding
he deg ada ion o OMPs allows kine ic imp o emen s e en when p e-
sen in ace amoun s [46]. The H₂O₂-media ed gene a ion o •OH can
consume up o hal he amoun o a ailable O₃ [47], he e o e, he H₂O₂/
O₃ a io is gene ally se be ween 0.5 and 1.0. A pilo and ull scale, he
eac ion is o en ca ied ou in gas-liquid eac o s wi h a con igu a ion
simila o ozone bubbling columns. Al e na i ely, he decomposi ion o
hyd ogen pe oxide in p esence o UV i adia ion leads he o ma ion o
addi ional •OH adicals [23,48]. Ca aly ic ozona ion (O₃₃-CAT) makes
use o a ca alys o p omo e he decomposi ion o ozone and he sub-
sequen o ma ion o ROS. Al hough many homogeneous ca alys s based
on ansi ion me al ions, p e e ably bi alen , ha e been in es iga ed,
p ecipi a ion o lack o e en ion sys ems ha e p e en ed hei la ge-
scale applica ion [49]. In he la e 1990s, he i s pilo plan s applied
he e ogeneous ca alys s o imp o e ozona ion e iciency in leacha e
ea men [50]. Applicable ma e ials a e i on lakes, me al/me al oxide-
coa ed ce amic memb anes o clay mine als such as mon mo illoni e
[49,51]. The applica ion o alumina-based ca alys s showed a signi ican
enhancemen o mic opollu an emo al compa ed o ozona ion alone
[52]. In con as , he applica ion o i on-based ca alys s o he emo al
o sul ame hoxazole showed no imp o emen compa ed o he esul s
wi h he esul s ob ained o con en ional ozona ion [53]. On he o he
hand, he possibili y o in eg a ing ozona ion wi h elec ochemical
me hods aims a he coagula ion o dissol ed me als [25] and will be
applicable o was ewa e s o high con en in hea y me als.
The combina ion o ozona ion wi h di e en ypes o ac i a ed ca -
bon such as GAC [54,55], biological ac i a ed ca bon (BAC) [56,57],
bio il a ion [38,55] o sand il a ion [43,58] has been success ully
applied. As an example, ¨
Os man e al. [59] epo ed he imp o emen in
benzo hiazole emo al om 30% o 82% by inco po a ing a GAC uni
a e he ozona ion s age. Howe e , in his s udy, he applica ion o sand
il a ion o his e luen did no show a signi ican e ec [56,58,59]. On
he o he hand, he use o biological il e s has been s udied by Knopp
e al. [55] and Te nes e al. [38], showing simila esul s o hose ob-
ained by he applica ion o ozona ion.
4.2. Ul a iole ea men s
Ul a iole (UV) i adia ion is commonly applied as disin ec ion
s ep a e biological ea men . UV uni s o disin ec ion usually consis
o cylind ical bo osilica e modules housing me cu y p essu e lamps
imme sed in he was ewa e s eam (Fig. 4A). Bo h low p essu e (LP)
lamps, wi h a sha p emission peak a abou 254 nm, and medium
p essu e (MP) lamps wi h a b oade emission spec um in he UV-C e-
gion (200–600 nm) a e applied. The low capaci y o hese ull-scale
modules can be up o 3000 m
3
h
−1
[60] in single-pass mode o a esi-
dence ime o less han 1 min. The in luen ea ed in he e ised s udies
was cha ac e ized by a pH in he ange o 7.0–7.6 and a empe a u e
anging be ween 18 and 24 ◦C, and compa ably low TSS and DOC alues
(Fig. 4B). Mos o he conside ed s udies we e pe o med in Eu ope, wi h
a concen a ion o he Medi e anean a ea, while he la ges plan s
ega ding ea ed low we e loca ed in China, only one s udy was in
B azil, ocusing on pa hogen emo al.
Pa hogen emo al by UV ligh ypically anges be ween 5 and 7 LRV
a i adiance le els o 70 W m
−2
. These high emo al alues a e
necessa y o mi iga e he e ec o bac e ial eg ow h a e UV ea men
[61]. This possibili y is o pa icula conce n when eclaimed was e-
wa e is s o ed in bu e anks p io o use o ag icul u al pu poses. I
should be no ed ha ce ain species o bac e ia show esis ance o UV
ea men . While he mos commonly in es iga ed E. coli bac e ia a e
S. de Boe e al.
Jou nal o Wa e P ocess Enginee ing 46 (2022) 102587
6
e ec i ely emo ed e en wi hin a sho esidence ime, Pseudomonas
s ains a e equen ly de ec ed in e luen om UV disin ec ion uni s
[42]. Rega ding he elimina ion o gene ic pa e ns ele an o he
e olu ion o an ibio ic esis ances, se e al s udies epo ed ha UV
ea men only selec i ely elimina es ARGs, and epo ed emo als o
DNA o gene agmen s was lowe han o pa hogens (ESM 6) [60,62].
Al hough many au ho s ha e s udied OMP emo al in ull-scale
modules designed o disin ec ion [63], hese app oaches only lead o
sligh emo al e iciencies o applied i adiances up o 500 mJ cm
−2
,
e en an i adiance o 4000 mJ cm
−2
only esul ed in a emo al o 0.77
LRV o mic opollu an s [64]. Simila emo al pe cen ages o endoc ine
dis up ing chemicals (EDCs) we e epo ed by C´
eda e al. [65] a i a-
diance o 1000 mJ cm
−2
. I was also shown ha es ogenici y could no
be sa is ac o ily emo ed, e en hough he pa en compounds we e
pa ially ans o med [66]. Rega dless o he lamp in ensi y in he
pho olysis p ocess, i is equi ed ha he a ge OMPs abso b he UV
adia ion in he ange o he lamp spec um o be aba ed. Howe e , only
a ew o ganic mic opollu an s p esen in was ewa e unde go pho olysis
a he applied wa eleng h o 245 nm. These a e, o example, sul a-
me hoxazole wi h a emo al e iciency be ween 22 and 70% [67],
depending on he applied i adiance [63,68,69] and diclo enac be ween
45% and 100% [61,68] (Fig. 4D). E en i he a ge molecule is no
suscep ible o pho olysis, i may unde go seconda y adical ans-
o ma ion p omo ed by ligh -induced exci a ion o elec ons om
compounds p esen in he ma ix. Gene ally, he s udies e iewed we e
ope a ed a dissol ed o ganic ca bon (DOC) alues below 15 mg L
−1
wi h ew excep ions. S ill, mos o he in es iga ed OMPs a e only
deg aded o a negligible ex en [70] o e en wi h nega i e emo al e -
iciencies [71,72]. This may be ela ed o se e al ac o s such as
pho olysis o coupling p oduc s owa ds he o iginal compounds, e o s
in quan i a i e measu emen s due o ma ix in e e ence o deso p ion
o esidual pa icula e ma e [66]. None o he in es iga ed s udies
conside he a e o hea y me als du ing UV ea men , as UV i adia ion
is known o ha e no e ec on hei emo al.
UV- ea men combined wi h hyd ogen pe oxide (UV-H₂₂O₂₂)
p oduces eac i e hyd oxyl adicals as ligh wi h wa eleng hs >254 nm
Fig. 4. A) Schema ic ep esen a ion o an ul a iole ea men uni . B) Wo ldwide dis ibu ion o he analyzed s udies (ci cle a ea is p opo ional o he ea ed low
a e and colo ep esen he ype o ea men –blue: UV, yellow: UV +H
2
O
2
, g een: UV+o he oxidan and ed: sola ea men –). C) O e iew o he quali y
equi emen s o he in luen and ypical ope a ional pa ame e s and consumables anges o he analyzed s udies. D) Remo al e iciencies o he mos in es iga ed
compounds (n >2). The ac onym lis is a ailable in Supplemen a y In o ma ion (ESM 3). G ey columns s and o UV +H
2
O
2
and whi e columns ep esen s and-
alone UV ea men esul s. (Fo in e p e a ion o he e e ences o colo in his igu e legend, he eade is e e ed o he web e sion o his a icle.)
S. de Boe e al.
Jou nal o Wa e P ocess Enginee ing 46 (2022) 102587
7
induces pho odissocia ion o H₂O₂ [70], esul ing in enhanced mic o-
pollu an emo al [73–75]. Typically, a H₂O₂ dose o 10 mg L
−1
is
applied in pho o eac o s equipped wi h dosing-mixing sys ems ha a e
al eady comme cially a ailable o la ge-scale applica ions [65,76].
Va ious eac o geome ies ha e been e alua ed o maximize mixing and
i adia ion [68]. Howe e , he bene i s o combining sunligh o UV
wi h hyd ogen pe oxide a e less p ominen o an ibio ic emo al and
disin ec ion [67]. Al hough H
2
O
2
is he mos used oxidan , i has been
shown ha he use o o he oxidan s conside ably minimizes bac e ial
eg ow h compa ed o UV ea men alone [61]. Rega ding OMP,
emo al e iciencies a e highly dependen on he ype o con aminan s,
so a iable ene gy e iciency alues we e ob ained, anging om
0.16–18 kW m
−3
o cip o loxacin and cla i h omycin, espec i ely
[10]. I is he e o e necessa y o e alua e and model he deg ada ion
kine ics o he expec ed mic opollu an s bo h in labo a o y and a pilo
scale [66,67,77]. O he oxidan s such as ozone, chlo ine, chlo ine
dioxide and pe sul a e in combina ion wi h UV ea men ha e been
also in es iga ed o OMP emo al [73–75]. Compa ed o •OH adicals,
Cl and SO₄
−
. adicals ha e been epo ed o be less p one o deac i a ion
by ma ix cons i uen s such as HCO₃
−
o NO₃
−
and o ha e less a ini y
owa ds na u al o ganic ma e [61,77]. The unde lying mechanisms o
adical o ma ion and eac ion wi h OMP a e desc ibed in de ail else-
whe e [78,79].
4.3. Adso p ion on ac i a ed ca bon
Al hough ad anced ma e ials such as zeoli es o ca bon nano ubes
a e gaining in e es as adso ben s in was ewa e polishing, ac i a ed
ca bon is used as he p edominan ma e ial, depending on he g ain size,
as powde ed ac i a ed ca bon (PAC) o g anula ac i a ed ca bon
(GAC).
Powde ed ac i a ed ca bon is applied in g ain sizes o 50–100
μ
m
wi h a BET su ace a ea be ween 900 and 1300 m
2
g
−1
[80]. PAC is
usually added o he e luen o he biological ea men s age in a
[81–83] loading ange be ween 10 and 20 mg L
−1
. One o he cons ain s
in he design o di e en p ocess con igu a ions mus ensu e he e en-
ion o spen PAC [84], achie ed by (1) he implemen a ion o a sedi-
men a ion uni [85,86] o by (2) sand, an h aci e o expanded shale bed
Fig. 5. A) Schema ic ep esen a ion o ypical con igu a ions o 1) GAC and 2) PAC p ocesses. B) Wo ldwide dis ibu ion o he analyzed s udies (ci cle a ea is
p opo ional o he ea ed low a e and colo ep esen he con inen ). C) O e iew o he quali y equi emen s o he in luen and ypical ope a ional pa ame e s
and consumables anges o he analyzed s udies. D) Remo al e iciencies o he mos in es iga ed compounds (n >2). The ac onym lis is a ailable in Supplemen a y
In o ma ion (ESM 3). G ey columns s and o GAC, and whi e columns s and o PAC ea men esul s.
S. de Boe e al.
Jou nal o Wa e P ocess Enginee ing 46 (2022) 102587
8
il e columns o , in some cases, by (3) memb ane il a ion uni s
(Fig. 5A). In he la e wo op ions, PAC ecycling can be achie ed by
backwashing o maximize he ca bon usage a e. Howe e , in he i s
case, i is necessa y o imp o e PAC e en ion by coagula ion-
loccula ion, which equi es he addi ion o Fe
3+
-based coagulan s
[83]. In some cases, an anionic polyme is addi ionally applied as a
locculan [85]. Al e na i es whe e PAC is di ec ly applied in memb ane
bio eac o s (MBR) may pose p oblems in sludge managemen [87] as
spen PAC is mixed wi h he sludge ma ix and canno be egene a ed
a e use. A p omising ad ance in p ocess simpli ica ion is he de el-
opmen o
μ
GAC, which is coa se and hus easie o sepa a e and
egene a e [88,89].
GAC uni s a e mainly applied con inuously in packed bed il e col-
umns (Fig. 5A), which ha e o be eplaced a e he b eak h ough
h eshold is eached. Se e al columns a e applied in se ies o in pa allel,
while each con igu a ion has d awbacks and ad an ages [90,91]. The
same applies o he il a ion di ec ion, ei he down low o up low,
which esul s in di e en head loss p o iles, while he emo al e iciency
was epo ed only sligh ly highe in he up low con igu a ion [90]. In all
cases, egula backwashing is equi ed o impede p essu e buildup and
can inc ease he ope a ion ime o he il e columns. Based on expe i-
ence du ing one yea o pilo scale ope a ion, Kå elid e al. [87] es i-
ma ed he main enance ime o be 30–60 min pe day. The mos c i ical
ac o s o he was ewa e ma ix ha a ec he s able pe o mance o
GAC il e s a e DOC and pH alue, hese alues a e be ween 6 and 11 mg
L
−1
(Q1-Q3) and 7.0–7.6 (Q1-Q3) espec i ely. TSS a e conside ed o
ha e a mino e ec on he emo al pe o mance o GAC il e s, bu high
le els equi e inc eased backwashing and ange om 3 o 6 mg L
−1
(Q1-
Q3) in he e iewed s udies [40,92] (Fig. 5B). Fig. 5C shows he
geog aphical dis ibu ion o he e ised s udies based on ac i a ed ca -
bon, indica ing a ocus o implemen a ion in cen al and Wes e n Eu ope
and he USA. This is explainable by he s ic e legisla ion ega ding he
p esence o OMP in WWTP e luen s implemen ed in Swi ze land and
local ini ia i es as in some Ge man ede al s a es (No h Rhine Wes -
phalia and Baden Wu embe g). Bo h PAC and GAC can be conside ed
as a s ong ba ie agains mos mic opollu an s [87,93].
Due o he nume ous GAC p oduc s a ailable, a iable was ewa e
composi ion, and complex in e ac ion mechanisms, a quan i a i e p e-
dic ion o ea men capaci y and GAC b eak h ough alues is no
s aigh o wa d and mus be pe o med on a case-by-case basis [89].
Ano he ac o ha adds complexi y o he desc ip ion o GAC p ocesses
and modeling o b eak h ough beha io is he de elopmen o a bio ilm
in he GAC bed o e a p olonged ope a ing ime, which ul ima ely u ns
hem in o BAC il e s [55]. While adso p ion- ela ed emo al e iciency
will dec ease du ing mic obial e olu ion, biodeg ada ion becomes mo e
ele an [40,94,95]. As expec ed in ela ion o he la ge su ace a ea, a
smalle GAC pa icle size is usually a o able o OMP emo al [59]. The
da a ob ained om he e ised s udies indica es ha he GAC p ocess
can achie e highe maximal emo als o all selec ed indica o com-
pounds, bu he da a is mo e sca e ed han in he PAC p ocess. Mos
c i ical compounds we e diazepam, alsa an, acesul ame K and sul a-
me hoxazole, while a enolol, beza ib a e and me op olol we e emo ed
>80% in mos s udies (Fig. 5D). In pa icula , highe pK
a
alues and
hyd ophobici y o OMP a o adso p ion on o nega i ely cha ged ac i-
a ed ca bon [22,94]. Depending on he ea men goals and quali y o
ea ed wa e , GAC p ocesses can be in eg a ed in o ea men ains, e.
g. GAC is o en used as a polishing s ep a e ozone/AOP ea men ,
combining he bene i o low DOC con en and he e icien emo al o
ozona ion/oxida ion byp oduc s.
4.4. P essu e-d i en memb ane il a ion ea men s
In e e se osmosis (RO) and nano il a ion (NF) p ocesses, wa e
is pumped h ough a a iable se o p essu ized memb ane elemen s,
yielding a ea ed pe mea e s eam and a concen a ed e en a e s eam.
The pe cen age o he pe mea e lux ega ding he in luen lux is
de ined as eco e y, anging be ween 50 and 90% [18]. High eco e ies
can be achie ed by applying wo consecu i e s ages, eeding he second
s age wi h e en a e om he i s s age, while highe pe mea e quali y
can be eached by a second pass h ough ano he s age (Fig. 6A). The
mos commonly applied polyme ic memb anes ha e a li e ime o abou
5 yea s, depending on he quali y o he ea ed wa e [96]. Recen ly,
ce amic memb anes a e gaining in e es despi e highe manu ac u ing
cos s due o hei longe li e ime, which can each a du a ion 20 yea s
[97,98]. In he e iewed s udies, he ope a ion o spi al wound poly-
me ic modules in c oss low con igu a ion is p e e ed o e la shee
con igu a ion, while memb ane a eas be ween 2.2 and 14.0 m
2
o pilo
scale [99,100] and be ween 1000 and 3000 m
2
o ull scale we e
in es iga ed. In bo h NF and RO p ocesses, p essu es in he ange o
7–15 ba a e applied, necessa y o o e come he memb ane esis ance
and he osmo ic p essu e be ween pe mea e and concen a e [18].
P essu e mus be ca e ully moni o ed, as i s sudden dec ease e lec s
memb ane damage, while con inuous inc ease in p essu e indica es
memb ane ouling/scaling due o he deposi ion o sal s, colloids and
o ganic ma e clogging he po es [101–103]. Despi e some excep ions
whe e TSS concen a ions we e up o 1800 mg L
−1
o pha maceu ical
e luen s [104] and 390 mg L
−1
o p ima y ea ed municipal was e-
wa e s [105], TSS and DOC le els a e lowe wi h maximum concen-
a ions o 15 mg L
−1
[96] and 30 mg L
−1
[106] espec i ely.
Conside ing he suscep ibili y o ouling, RO and NF sys ems a e usually
p eceded by an ul a il a ion (UF) module o a memb ane bio eac o
(MBR). High wa e empe a u es (>30 ◦C) usually lead o a dec ease in
memb ane pe o mance [107,108] (Fig. 6B) Despi e he limi a ions
imposed by in luen quali y, he implemen a ion o RO/NF as an al e -
na i e o seconda y biological ea men has al eady been applied as a
decen alized ea men solu ion o p oduce high quali y e luen [105].
Ne e heless, he main applica ion a la ge scale is wa e eclama ion in
he ange o 150,000–450,000 m
3
d
−1
in egions wi h high wa e sca -
ci y [109]. The s udies conside ed in his e iew we e pe o med a
smalle scale plan s which anged om 50 o 180 L h
−1
(pilo ) [96,110]
and 24–168 m
3
d
−1
( ull scale) [105,111]. A ele an sha e (39%) o he
s udies e iewed in ou wo k we e conduc ed in Spain, while s udies
we e dis ibu ed wo ldwide, including s udies om Sou h A ica, B azil,
and India (Fig. 6C).
Focusing on he g oup o a ge con aminan s, he mos s udied
compounds in he e iewed publica ions a e ca bamazepine (CBZ),
ca eine (CAF), diclo enac (DFC), ibup o en (IBU) and sul ame hoxazole
(SMX) a e p esen ed in Fig. 6D. The emo al e iciency o bo h ech-
nologies is simila o he analyzed pollu an s, excep o ca bamaze-
pine, o which RO p o ed mo e e ec i e. Re en ion o OMP is mainly
go e ned by size exclusion, howe e se e al ac o s such as hyd opho-
bici y, su ace loading o con aminan s, o bio ilm o ma ion can posi-
i ely in luence e en ion [111]. Al hough mos s udies epo excellen
emo al o OMP (e.g., sul ame hoxazole, diclo enac, ibup o en and
a enolol) below he de ec ion limi , his is no he case o some com-
pounds, especially o small molecula weigh [112]. Fo example, he
small endoc ine dis up o bisphenol-A o ni osamines, such as N-
ni osodime hylamine (NDMA), and o he ozona ion/AOP byp oduc s
a e equen ly ound in RO pe mea es [111,113]. In his ega d, i may
be bene icial o apply RO/NF s ages p io o AOP p ocesses, as i has
been shown ha NDMA p ecu so s such as ani idine can be e icien ly
emo ed by NF and RO [114]. I should be no ed ha lowe concen-
a ions o OMP a e mo e di icul o emo e possibly due o slowe
eac ion a es and/o ma ix e ec s [112], which also emphasizes he
need o in es iga ions a en i onmen al concen a ions in o de no o
o e es ima e he e iciency o he p ocess. Resea ch s udies a ely ocus
on pa hogen emo al by RO and NF s ages, as hey a e usually p eceded
by an ul a il a ion uni o a oid bio ilm g ow h. Al hough ul a il a-
ion memb anes a e a su icien ba ie agains bac e ia, i uses and
OMPs a e only su icien ly e ained by NF and RO memb anes [96,115].
NF and RO a e also e ec i e o hea y me al emo al, bu his ea u e is
only ele an in special applica ions, e.g. highly con amina ed land ill
S. de Boe e al.
Jou nal o Wa e P ocess Enginee ing 46 (2022) 102587
9
leacha e o cons uc ion si e e luen s [116,117], since hea y me als in
municipal e luen s a e mos ly success ully e ained in seconda y bio-
logical ea men .
4.5. Ca alys -based p ocesses
Ins ead o di ec ly using pho on ene gy o decompose mic opollu an
s uc u es, ROS a e o med du ing pho oca aly ic p ocesses using ma-
e ials wi h semiconduc ing p ope ies o based on ligh -d i en
decomposi ion o hyd ogen pe oxide (pho o-Fen on). Due o he
highe ene gy equi emen s o UV ligh compa ed o sola ligh , ecen
wo k ocuses on he sea ch o new ma e ials capable o exploi ing he
ad an ages o his ype o i adia ion wi h a ocus on educing ene gy
consump ion esul ing in g ea e echnological easibili y o la ge-scale
implemen a ion (Fig. 7A). In pho oca alysis p ocesses, app oxima ely
hal o he s udies ha e used sola ligh and p o ide i adiance be ween
20 and 40 W m
−2
in lowe la i ude a eas [118–120]. The mos applied
echnologies we e pilo aceway pond eac o s (RPR) o compound
pa abolic eac o s (CPR). While he s udied RPR eac o s ha e an illu-
mina ed a ea o less han 0.5 m
2
and a dep h o 5 o 15 cm o cope wi h a
wo king olume o abou 20–100 L [120–122], he la ges pilo CPC
plan s o was ewa e ea men ha e a ea men capaci y a ound 100 L
in ba ch ope a ing mode [123–125]. The mos equen pa ame e s
s udied wi h hese echniques we e depic ed in Fig. 7B.
He e ogeneous pho oca alys s (PC) in was ewa e ea men a e
based on he use o solid-s a e me al oxides wi h semiconduc ing p op-
e ies. In hese ma e ials, he alence and conduc ion bands (VB and CB)
a e sepa a ed by an ene gy band gap. Upon i adia ion o pho ons wi h
an ene gy equal o o highe han his ene gy, elec ons in he VB a e
p omo ed o he CB. The o ma ion o elec on-hole pai s p o ides si es
o he gene a ion o ROS by oxida ion and educ ion eac ions, ac ing as
di ec oxidan when an o ganic molecule se es as an elec on dono , o
as indi ec oxidan by gene a ion o •OH which in u n a acks o ganic
molecules [126]. In heo y, o ganic mic opollu an s could be comple ely
mine alized as he adical eac ions a e non-speci ic and a e capable o
deg ading a wide ange o compounds, howe e , he gene a ion o by-
Fig. 6. A) Schema ic ep esen a ion o di e en con igu a ions o memb ane il a ion uni : wo-s age (g een line bounda y) and wo-pass con igu a ion (blue line
bounda y). B) Wo ldwide dis ibu ion o he analyzed s udies (ci cle a ea is p opo ional o he ea ed low a e and colo ep esen he con inen ). C) O e iew o
he quali y equi emen s o he in luen and ypical ope a ional pa ame e s o he analyzed s udies D) Remo al e iciencies o he i e mos in es iga ed compounds
o nano il a ion and e e se osmosis s udies. G ey columns s and o RO and whi e columns s and o NF ea men esul s. (Fo in e p e a ion o he e e ences o
colo in his igu e legend, he eade is e e ed o he web e sion o his a icle.)
S. de Boe e al.
Jou nal o Wa e P ocess Enginee ing 46 (2022) 102587
16
al e na i e pos - ea men s o a PAC p ocess, showing ha he p ocess
cos s wi h he implemen a ion o nano il a ion comp ised 0.80
€
m
−3
while sand il a ion accoun ed only o 0.16
€
m
−3
. Eche a ía e al.
[238] epo ed an OPEX o 0.31
€
m
−3
o a plan size o 15,000 m
3
d
−1
while assuming a memb ane li e ime o 6 yea s and ene gy consump ion
o 1.3 kWh m
−3
. The CAPEX accoun ed o 662
€
m
−3
d
−1
( ansla ing o
0.044
€
m
−3
a peak low). When ea men goals a e less s ingen , a
common op ion o cos educ ion is o di e he low o was ewa e ,
mixing wi h RO ea ed wa e . By p oducing a 50% blend, he OPEX
could be educed o 0.18
€
m
−3
on he expense ha emo al o selec ed
OMP is educed o 50%. Fu he mo e, since he ene gy demand o
pumping scales almos linea ly wi h memb ane a ea and applied p es-
su e, he size o he plan does no signi ican ly educe ope a ing cos s.
Ga cia e al. [96] calcula ed OPEX eaching 0.24
€
m
−3
while CAPEX
dec eased om 0.48–0.31
€
m
−3
compa ing ea men capaci ies be-
ween 1 and 1000 ML d
−1
. Con e sely, Hube e al. [239] a gued ha he
a he simple con igu a ion o memb ane il a ion can lead o low
capi al cos s compa ed o o he ea men s. Thi y-nine pe cen o he
e iewed s udies in es iga ing memb ane ea men s we e conduc ed in
Spain, while he es o he s udies we e dis ibu ed wo ldwide,
including publica ions om Sou h A ica, B azil and India. In con as ,
only one pilo -scale s udy was p esen ed o Ge many [240]. This can be
explained by he disc epan ene gy cos s [241], as in 2020 household
elec ic ene gy p ices we e 0.08 $ kWh
−1
in India, he p ice in Ge many
was 0.38 $ kWh
−1
. Recen ly, he possibili y o using ene gy-in ensi e
bu lexible p ocesses, such as e e se osmosis, as a bu e in ene gy
g ids inc easingly based on ex ac able ene gy has been p oposed.
Flexible ope a ion pa e ns o WWTPs could compensa e o he luc-
ua ing p oduc ion capaci y o wind and sola ene gy [242].
Elec ochemical ea men s a e usually ega ded as ene gy in en-
si e ea men s. Al hough elec ochemical ea men s, such as elec o-
oxida ion, p esen high ene gy consump ions [76], he use o
elec ochemical-assis ed echniques p esen s compe i i e ope a ional
cos s o be implemen ed in WWTPs. The use o elec odialysis is op i-
mized by i s ex ensi e use in desalina ion and can be an e ec i e me hod
o emo e hea y me als. Fo ins ance, a pilo plan wi h a p oduc i i y o
285 m
3
h
−1
in eg a ing elec odialysis in a ea men ain wi h ul a-
il a ion and e e se osmosis a ained excellen educ ion o coppe
concen a ion wi h an es ima ed o al cos o 0.3–0.4
€
pe m
3
o ea ed
wa e [243]. The use o elec ochemical echnologies o he elec o-
gene a ion o H
2
O
2
is also epo ed o educe he cos s compa ed o
dosage. Fo ins ance, Wang e al. [100] es ima e ha he ene gy
equi ed o he in-si u gene a ion o H₂O₂ accoun s o addi ional cos s
o be ween 0.4 and 0.8 USD kg
−1
, while he dosage o H₂O₂ in ol es
cos s o 1.2–1.5 USD kg
−1
.
Fo o he inno a i e ea men s, he e is a lack o a ailable da a o
cos calcula ions, as only labo a o y-scale da a a e a ailable. The ene gy
consump ion o UV-pho oca alysis, ul asound and mic owa e pho o-
ca alysis ea men s ha e been epo ed o exceed e en 100 kW m
−3
,
howe e , calcula ions on his basis end o o e es ima e ene gy con-
sump ion and hus cos s [229]. Inc easing ene gy e iciency wi h
inc easing plan size is a common concep in s udies conside ing p ima y
o seconda y ea men plan s. In he sho - e m pe spec i e, hese
ea men op ions ha e po en ial o be u he applied and in es iga ed
o he ea men o highly con amina ed indus ial was ewa e , land ill
leacha e and RO/NF e en a es. Fo example, he highe o e all ea -
men cos s o land ill leacha e, e en wi h con en ional ea men s, and
he ypically lowe olumes ea ed, open up mo e op ions o he
applica ion o inno a i e ea men p ocesses.
In e ms o he cos s and impac s o each echnology, use s and
egula o s mus ca e ully balance he amoun o in es men , bo h eco-
nomic and en i onmen al, o achie e he goal o sa e wa e esou ces.
Mu˜
noz e al. [244] p opose an in eg a ed app oach o assess he eco-
e iciency o a echnology by weighing en i onmen al and economic
bu dens. Based on hei easoning, ozona ion was less a o able han
pho o Fen on o sola pho o Fen on ea men . Howe e , he cos s
assumed in his s udy we e almos en o de s o magni ude highe han
in he s udies e iewed abo e. The cen alized and dis ibu ed appli-
ca ion o e ia y ea men s was also s udied o se e al es ablished
echnologies. Acco ding o he esul s, cen alized ea men is p e e ed
o he disposal o pha maceu icals [184], bu mo e esea ch would be
needed o con i m his. In addi ion, social aspec s will play a conside -
able ole in he inal s eps o decision-making. In Swi ze land, he public
suppo ed he decision o legally oblige WWTPs o gua an ee he
emo al o ce ain indica o pollu an s a 80%. This measu e will in-
c ease ea men cos s by 6% ac oss he coun y. In addi ion, ene gy
consump ion is es ima ed o inc ease by a ound 0.1% wi h he mos
ad anced echnologies [237,245]. Howe e , de eloping coun ies will
no ha e he esou ces o implemen such p og ams in he nea u u e, as
he p io objec i e is s ill o p o ide a leas adequa ely disin ec ed
wa e . Despi e his di icul si ua ion, he lack o in as uc u e ne wo ks
could also lead o he de elopmen o simple decen alized ea men
op ions based on enewable ene gy sou ces mo e quickly han in
de eloped coun ies.
7. Benchma king o he echnologies
As a as sa e wa e euse s a egies a e conce ned, he e ia y
ea men p ocesses applied mus ul il se e al amewo k condi ions.
The ea men ains mus be adap able in size o he was ewa e low
and pollu an load a he espec i e applica ion si e, while ope a ion has
o be eliable and p o ide edundancy in case o ailu e o indi idual
uni s. The e o e, ep oducible measu emen schedules o indica o
subs ances should be suppo ed by as online moni o ing echniques
such as luo escence exci a ion emission ma ices (FEEM), as well as by
e ec -based assays on (acu e) oxici y, es ogenici y, mu agenici y o
an ibio ic suscep ibili y [246]. The in eg a ion o easonable and s an-
da dized p o ocols in a “whole e luen ” app oach is cu en ly an
impo an esea ch opic [247]. A sound assessmen o he (a oided)
isks o each echnology is he basis o a comp ehensi e LCA s udy.
Fu he mo e, egionaliza ion o cha ac e iza ion ac o s was sugges ed
as a key issue o ep esen an accu a e oxici y impac in local en i-
onmen s [248]. I is also epo ed ha he cu en ly used assessmen
me hods could p o ide di e en esul s and may no include some
mic opollu an ac o s [249].
In he ollowing we summa ize and quali a i ely discuss he main
s eng hs and weaknesses o each ad anced ea men echnology unde
echnological, en i onmen al and economic poin s o iew, based on he
indings o he s udies selec ed. The echnologies e iewed can be
classi ied in o (ad anced) oxida ion p ocesses and physical e en ion
ea men s. While oxida ion p ocesses comp ise adi ional ozone
ea men and eme ging ancilla y echnologies, con en ional UV ea -
men and enhancemen echnologies, as well as elec ochemical ea -
men s, physical ea men s include adso p ion p ocesses mainly based
on ac i a ed ca bon and memb ane il a ion (Table 1).
One o he main d awbacks o ozona ion is ha , due o i s high
eac i i y and ins abili y, ozone mus be gene a ed on-si e om oxygen
by elec ical discha ge, wi h a yield o abou 10%, which leads o high
elec ical ene gy consump ion in he plan . In addi ion o he low ozone
yield, he e ec i eness o ozone ea men is limi ed by i s slow disso-
lu ion a e and apid decomposi ion. Howe e , modi ica ions o ai
di use s ha o m mic o-nano bubbles inc ease he ea men e iciency
[46]. Fu he mo e, he high oxici y o ozone equi es he design o
ozone des uc ion uni s which emo e un eac ed ozone om he exhaus
gas s eam a e ea men [250]. T ained pe sonnel and s ic sa e y
p o ocols a e necessa y o minimize he isk o acciden al elease. In
addi ion, he o ma ion o oxic by-p oduc s such as b oma es, which a e
po en ial human ca cinogens, has been associa ed wi h his p ocess
[251]. Inc eased e luen oxici y a e ozone ea men was epo ed by
se e al s udies and con ibu ed o wo sen en i onmen al impac s om
an LCA pe spec i e. Despi e hese d awbacks, disin ec ion capaci y and
low ope a ional cos s a e he main ad an ages o ozona ion [252]. The
S. de Boe e al.
Jou nal o Wa e P ocess Enginee ing 46 (2022) 102587
17
de imen al e ec s o induced oxici y can be ci cum en ed when an
addi ional il a ion/adso p ion s ep is applied a e ozona ion. In e ms
o applicabili y o was ewa e ma ix condi ions, DOC is he mos c i ical
cons i uen ha needs o be con olled p io o ozona ion, while o he
cha ac e is ics such as TSS o u bidi y ha e a mino in luence as hey
a e no ela ed o DOC. The lowes emo al a es we e ob ained o
ibup o en, oxazepam and suc alose, and hei emo al could be
analyzed in he e alua ion o ope a ional condi ions o inc ease he
sensi i i y o he me hod. Fu he esea ch should ocus on in es iga ing
e luen oxici y, elimina ion o an ibio ic esis ance genes, and decision-
making based on ope a ional cos s and en i onmen al impac .
Con en ional UV ea men o pa hogen emo al equi es i adi-
ances o <500 mJ cm
−2
and sho esidence imes, esul ing in ela i ely
low cumula i e ene gy doses ha minimize ope a ing cos s. Howe e ,
hese con igu a ions a e no e icien o OMP emo al, no only because
o he low ans e ed ene gies bu also because o he in insic ecal-
ci ance o mos OMPs o di ec UV pho olysis. The i s obs acle has
been o e come wi h he de elopmen o high in ensi y pho o eac o
modules. To add ess he second p oblem, he dosing o addi ional oxi-
dan s has p o en e ec i e. While hyd ogen pe oxide in combina ion
wi h high in ensi y UV ea men is al eady applied on a la ge scale,
pe sul a e and chlo ine dioxide a e s ill unde in es iga ion, especially
ega ding he o ma ion o oxic by-p oduc s. In addi ion, he en i on-
men al impac o hei p oduc ion and he possible isks associa ed wi h
hei unin en ional elease mus be conside ed. All UV-based p ocesses
equi e wa e wi h low u bidi y o maximize ansmi ance, so UV is
usually applied a e a cla i ica ion/ il a ion s ep.
Among he ca alys -based echnologies, Fen on-based me hods a e
he mos s udied. Howe e , he e is ag eemen ha he wo king pH o
Fen on-based me hods is a clea d awback, as chemicals a e used bo h
o acidi ica ion o he e luen and o pH co ec ion be o e discha ge o
euse. This d awback should be sol ed by imp o ing he eac ion a
neu al pH o see i s eal use in WWTPs. F om an en i onmen al poin o
iew, al hough he ope a ional phase has wo se impac s, Fen on-based
me hods could ha e less impac s i he cons uc ion phase is
conside ed. He e ogeneous p ocesses a e a o able compa ed o ho-
mogeneous p ocesses due o he easy eco e y o he ca alys and he
a oidance o changes in wa e composi ion. In addi ion, esea ch
ocused on he de elopmen o new ma e ials capable o imp o ing ligh
u iliza ion, combined wi h a eusable ca alys ope a ing unde ci cum-
neu al condi ions, should be he main p io i y o u he esea ch wo k
in his ield. In ela ion o he high en i onmen al impac o me cu y
p essu e lamp manu ac u ing, al e na i e i adia ion sou ces should be
in es iga ed. Al hough UV-LED i adia ion is p omising [253], i does
no ye each he ene gy e iciency o con en ional lamps and canno ye
be conside ed an economically iable al e na i e. Mo eo e , acco ding
o a ailable da a, di ec use o sunligh is mo e likely o emain a
p ospec o decen alized plan s in he medium e m. Howe e , he
indi ec use o sola ene gy h ough pho o ol aic plan s could be an
al e na i e wo hy o conside a ion in emo e a eas [254].
Bo h GAC and PAC adso p ion s ages a e e ec i e agains o ganic
mic opollu an s, howe e , hey do no achie e eliable emo al o hea y
me als, pa hogens and ARGs. In di ec compa ison o GAC wi h RO, a
simila ange o OMP was emo ed by GAC, bu RO was mo e e icien in
emo ing hea y me als and ola ile o ganic compounds [115]. In e ms
o on-si e ene gy demand, GAC sys ems a e p e e able compa ed o
ene gy-in ensi e p ocesses such as memb ane il a ion and ozona ion.
Howe e , when p oduc ion is included in he assessmen , GAC can be
mo e ene gy in ensi e han ozona ion, especially when adequa e ecy-
cling sys ems a e no applied. End-o -li e scena ios also ha e a high
en i onmen al impac [256]. Depending on he ea men goals, GAC
p ocesses can be in eg a ed in o ea men ains o e icien ly exploi
he bene i s o his ea men s age, o example, when a ge ing highe
OMP emo al in seconda y e luen s wi h high DOC loading, GAC can be
used as a polishing s ep a e ozone/AOP ea men [40,92]. In he case
o PAC, ecycling o spen adso ben is cu en ly no possible in mos
applica ions. In e ms o imp o ing he economic and en i onmen al
impac o PAC, no only e icien eci cula ion and ecycling schemes
need o be u he in es iga ed, bu he ma e ials applied mus be
enewable and no o ossil o igin. In he sho e m, ecycling o
Table 1
Quali a i e classi ica ion ma ix o he in es iga ed e ia y ea men s ega ding di e en easibili y c i e ia.
Ca ego ies
Oxida ion
Elec o
Adso p ion
Fil a ion
■Supe io pe o mance
■Baseline echnology
■Poo pe o mance
O3
UV/sola ligh
Elox
EC
GAC
PAC
NF
RO
O3
Ca
UV
H₂O₂
UV
PC
F/PF
H₂O₂
OMP emo al
Hea y me al emo al
Pa hogen emo al
Addi i es
Byp oduc s
Was e
Tu bidi y
pH
TSS
DOC
Ene gy demand
a
a
Ope a ional isks
Ope a ional cos s
a
On-si e ene gy demand.
S. de Boe e al.
Jou nal o Wa e P ocess Enginee ing 46 (2022) 102587
18
indus ial was e such as ly ash om coal plan s could also be a possi-
bili y [257]. Spen ac i a ed ca bon sludge mus be p ope ly handled o
p e en soil and su ace wa e con amina ion. Resea che s a e cu en ly
in es iga ing he ac o s in luencing OMP emo al by ac i a ed ca bon
p ocesses, as well as he applica ion o con ol s a egies, in o de o
inc ease he eliabili y o hese p ocesses.
Re e se osmosis and nano il a ion p ocesses an e icien ba ie
o e ain mos OMP, pa hogens (including ARGs) and hea y me als.
Depending on he con igu a ion, desalina ion can be achie ed, which is
an impo an ea men objec i e, especially in euse applica ions, and
esul s in a clea bene i o his echnology compa ed o o he s unde
e iew om which only elec odialysis is a conside able al e na i e o
sal emo al. The p oduced wa e can be p o ided wi h a eliable high
quali y, p o ided ha a p ope con ol and main enance p o ocol is
applied. Main enance ensu es he p ese a ion o he expensi e mem-
b ane modules agains ouling and scaling, bu equi es backwashing
p ocedu es wi h an i oulan s and an iscalan s, which con ibu es nega-
i ely o he en i onmen al impac . Al hough he RO/NF p ocess is well
es ablished in egions wi h high wa e s ess and compa a i ely low
ene gy cos s, om an LCA pe spec i e, e e se osmosis is no ecom-
mended by any o he a icles e iewed in his s udy, as he high ene gy
consump ion s ongly impac s en i onmen al indica o s such as g een-
house gas emissions. Resea ch should be di ec ed owa ds he de el-
opmen o mo e du able and e icien memb anes. This could lead o
lowe memb ane and ene gy cos s, as well as lowe consump ion o
cleaning agen s and hus lowe en i onmen al impac . Fu he mo e, he
gene a ion o a was e s eam in he ange o 10–20% o he o iginally
ea ed s eam inc eases he en i onmen al bu den and dec eases he
ea ed wa e yield [258]. Possible solu ions o he managemen o
e en a e a e i s eci cula ion o WWTP headwo ks, e apo a ion ponds
o AOP ea men s [259]. Fo smalle olumes and highe in insic
conduc i i y, elec ochemical oxida ion seems a p omising app oach
[141].
Elec ochemical me hods ha e g ea po en ial o educe he en i-
onmen al impac s associa ed wi h mic opollu an emo al, as hey
mainly use elec ici y, which can be conside ed as a clean chemical.
Howe e , pilo -scale esea ch is s ill sca ce, and he di e en echnol-
ogies need o each la ge scales o implemen a ion in a signi ican
numbe o publica ions o consolida e his po en ial. As highligh ed in
he LCA sec ion, ene gy and chemical p oduc ion a e esponsible o
mos o he en i onmen al impac s in e ia y ea men . Elec o-
chemical ea men s could he e o e be one o he keys in he ques o
educe chemical consump ion. Fo example, elec ooxida ion does no
use any chemical eagen s, while elec o-Fen on p ocesses p oduce H₂O₂
by elec o educ ion o oxygen. As o ene gy consump ion, elec o-
chemical sys ems can be easily combined wi h enewable ene gy sou -
ces, bu mo e s udies a e equi ed o op imize he coupling [260]. The
in eg a ion o enewable ene gy sou ces in combina ion wi h elec o-
chemical was ewa e ea men s is p o en o educe he en i onmen al
impac s p oduced by ene gy consump ion [222].
8. Concluding ema ks
One o he d awbacks o he p esen ed s udy is ha pee - e iewed
esea ch a icles a e a limi ed sou ce o ope a ional da a, gi en hei
speci ic ocus and basic p ocess pa ame e s such as uni dimensions,
c i ical con en ional was ewa e pa ame e s and low a es a e no al-
ways epo ed. Rega ding he apidly e ol ing esea ch on e ia y
ea men schemes, mo e e o should be made in publishing eliable
p ocess- ela ed da a in he pee - e iewed li e a u e. Ne e heless, he
o e iew p esen ed on he s a e o he a o e ia y ea men s clea ly
iden i ies he key poin s o bo h ull-scale p ocesses al eady ope a ed
and inno a i e ea men p ocesses based on hese con igu a ions and
p esen s he solu ions cu en ly unde de elopmen . To mee he e-
qui emen s o wa e sa e y s anda ds, a combina ion o di e en p o-
cesses (mul i-ba ie app oach) is o en essen ial o each indi idual
case.
In addi ion o economic and echnological conside a ions, en i on-
men al cons ain s iden i ied by a li e cycle assessmen mus be inco -
po a ed in o decision-making. Many au ho s poin ou ha he key
issues o mos e ia y ea men s a e he elec ical ene gy and chem-
icals consump ion. Mo e e o needs o be de o ed o he cha ac e -
iza ion o he ans o ma ion p oduc s p oduced in he ea men s o
accu a ely assess he impac o he me hods. The a iabili y o in luen
quali y needs o be moni o ed o ake ad an age o he high adjus abili y
o chemicals and added ene gy in he AOP, which will educe p ocess
cos s. Risks o pe sonnel and he en i onmen should be assessed p io o
implemen a ion. Fo a comple e isk assessmen , which is necessa y o a
sound li e cycle assessmen , mo e a en ion should be paid o p ocess
e alua ion based on oxicological da a han o deg ada ion e iciency
alone. Howe e , since so a , he applica ion o e ec -based e luen
con ol is s ill unde in es iga ion, ea men e icacy is egula ed and
compa ed based on indica o subs ance emo al a ge s. Many au ho s
a gue ha he low concen a ions o mic opollu an s and he lack o
sys ema ic assessmen o hei long- e m e ec s when eleased in o he
en i onmen mean ha he en i onmen al impac o new ea men
ains ou weighs he impac s o mic opollu an discha ge in o he
en i onmen .
Faced wi h his p oblem, mo e en i onmen al s udies a e needed o
be e unde s and he en i onmen al p o iles o e ia y ea men s,
p e e ably unde eal was ewa e condi ions and on a la ge scale, o
op imize cons uc ion and ope a ion da a, especially ene gy and
chemical consump ion. In addi ion, mo e wo k is needed on he analysis
o inno a i e e ia y echniques, as he analyzed e alua ions p o ided
some con adic o y esul s. In pa allel, he cha ac e iza ion ac o s o
mic opollu an s need o be e ised and alida ed, o imp o e he accu-
acy o LCA esul s o e luen s con aining hese pollu an s.
Supplemen a y da a o his a icle can be ound online a h ps://doi.
o g/10.1016/j.jwpe.2022.102587.
A ailabili y o da a and ma e ial
All da a gene a ed o analyzed du ing his s udy a e included in his
published a icle [and i s supplemen a y in o ma ion iles].
Funding
This esea ch was suppo ed by HP-NANOBIO (PID2019-111163RB-
I00) and SPOTLIGHT (PDC2021-121540-I00) p ojec s, g an ed by
Spanish Minis y o Science and Inno a ion.
CRediT au ho ship con ibu ion s a emen
Li e a u e sea ch, da a analysis and o iginal d a p epa a ion: Sab-
ina De Boe , Jo ge Gonz´
alez-Rod íguez and Julio J. Conde; Idea and
c i ical e ision: Ma ia Te esa Mo ei a.
Decla a ion o compe ing in e es
The au ho s decla e ha hey ha e no known compe ing inancial
in e es s o pe sonal ela ionships ha could ha e appea ed o in luence
he wo k epo ed in his pape .
Acknowledgemen s
S.d.B. hank ully acknowledges unding by he Eu opean Union's
Ho izon 2020 esea ch and inno a ion p og am unde Ma ie
Sklodowska-Cu ie g an ag eemen No 81288. J.G.-R. hanks Xun a de
Galicia Counseling o Educa ion, Uni e si ies and Voca ional T aining
(ED481A-2019/172) and Spanish Minis y o Science, Inno a ion and
Uni e si ies (FPU19/00461) o his p edoc o al ellowships. J.J.C. was
suppo ed by a pos doc o al ellowship om Xun a de Galicia (ED481B-
S. de Boe e al.
Jou nal o Wa e P ocess Enginee ing 46 (2022) 102587
19
2021/015). The au ho s belong o he Galician Compe i i e Resea ch
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