1
Ene gy Reco e y om E luen s o Supe c i ical Wa e Oxida ion
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Reac o s
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Yoana Ga cía-Rod íguez, Fidel A. Ma o*, Alexand a Ma ín, M. Dolo es Be mejo and
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M. José Coce o
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High P essu e P ocesses G oup, Depa men o Chemical Enginee ing and
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En i onmen al Technology. EII Sede Me gelina. Uni e si y o Valladolid. 47011
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Valladolid, SPAIN
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* Co esponding au ho , TEL: +34-983423169, e-mail: [email p o ec ed]
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Abs ac
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Supe c i ical Wa e Oxida ion (SCWO) eac o s can p ocess was e e luen s achie ing high
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con e sions, bu he equi ed ex eme p essu e and empe a u e ope a ional condi ions en ail
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high-ene gy ope a ional expendi u e. SCWO has he po en ial o be conside ed a clean ene gy
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gene a ion p ocess, as he p ocess e luen is a high empe a u e, high p essu e s eam wi h a high
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en halpy con en ha can be con e ed o hea and sha wo k. This ensu es he sel -sus ained
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eac ion and can gene a e excess sha powe o d i e bo h he high-p essu e pump and he ai
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comp esso . On he con a y, an e icien hea and powe eco e y om SCWO eac o s ou le
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s eams using con en ional p ocedu es p esen s se e al p oblems. Fi s , Rankine cycles impose
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indi ec hea ans e o he wo king luid and a e unable o eco e he p essu e ene gy and
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second, di ec expansion o he e luen s en ails cos ly de elopmen o speci ic, e icien
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expansion equipmen .
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In his wo k, we in es iga e he op ions o ene gy eco e y o SCWO eac o s coupled wi h
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comme cial gas u bines (GT). SCWO ou le s eams a e mainly composed o wa e , ni ogen and
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ca bon dioxide. These ope a ing alues nea ly esemble he well-known and al eady-implemen ed
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GT s eam injec ion p ocedu es. The empe a u e o he lue gases (app ox. 500 ºC) and he di ec
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sha wo k usage o e s adequa e ene gy in eg a ion possibili ies o bo h eed p ehea ing and
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comp ession. The wide ange o comme cially a ailable GT sizes enables p ocess scaling.
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Keywo ds: SCWO, sha wo k, ene gy eco e y, gas u bine (GT), s eam injec ion,
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simula ion.
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3
1. In oduc ion
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Supe c i ical Wa e Oxida ion (SCWO) is an in ensi e ene gy p ocess o elimina e
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o ganic was es. Fo many yea s he p ocess has been de eloping echnical solu ions o
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achie e esul s o co osion and plugins p oblems [1, 2]. Al hough i s indus ial
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de elopmen p og esses slowly, in 2013 wo indus ial plan s o chemical weapons and
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sludge ea men we e unde cons uc ion [3].
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One o he SCWO challenges is he ene gy eco e y o ge sha wo k and hea in
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o de o ge ne ene gy [4]. Exis ing li e a u e on SCWO p ocess ocusing on clean ene gy
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p oduc ion has been e iewed. Mos o he p ac ical de elopmen is based on eco e ing
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he hea eleased by was e oxida ion and gene a ing s eam. Many heo e ical wo ks poin
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ha he p ocess would be much mo e e icien i he comp ession ene gy could be
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eco e ed as wo k. The e icien he mal and p essu e ene gy eco e y will open he
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oppo uni y o use SCWO as an e icien and clean ene gy p oduc ion p ocesses om
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was es o biomass [5].
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Depending on he SCWO p ocess di e en al e na i es can be applied o hea
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eco e y. Con en ional ubula eac o s a e hin ubes, wi h e iden plugging p oblems
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om solid p ecipi a ion. In p ac ice, indus ial plan s wo k wi h wo eac o s, one unde
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ope a ion and he o he unde aking he cleaning o deposi ed solids. E en isola ed ubula
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eac o loss ene gy by he long su ace a ea, and u he mo e cleaning is a highly ene gy
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and ime consuming s ep. These eac o s can ope a e wi h ai o oxygen, bo h al e na i es
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wo k p ope ly. Oxygen is he mos usual oxidan o educe he ene gy consump ion o he
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ai comp esso . The oxida ion by oxygen equi es lowe eac o olume and less wo k o
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comp ess he liquid oxygen han he gas ai , bu he oxygen cos is he limi issue. The
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elec ion depends on he economic balance. Fo ope a ion below igni ion empe a u e,
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4
eac ion ime is abou se e al minu es and he eac o olume is minimized by he use o
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oxygen. Ai is mo e con en ional oxidan bu equi es highe eac o olume associa ed
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o ni ogen. To implemen he use o ai as oxidan he eac o olume could be minimized
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by he use o as e kine ic and by eco e ing he ene gy associa ed o he comp ession i
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he wo k om e luen dep essu iza ion could be e ie ed by a u bine.
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The eac o e luen ene gy can be eco e ed by a Closed Rankine Cycle h ough
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indi ec hea ans e o a wo king luid bu he p ocess is s ill highly ene gy demanding
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[6].
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Fo ope a ion a empe a u es abo e he igni ion, supe c i ical wa e oxida ion wi h
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hyd o he mal lame as in e nal hea sou ce allows o use ai o oxygen and he as e
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kine ics minimizes he eac o olume. The ope a ion unde hyd o he mal lames allows
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o al oxida ion o he was e wi hin milliseconds esidence imes, which opens he
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possibili y o de eloping small combus o s o p oduce high-p essu e gas/ apo s eams.
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The applica ion o hyd o he mal lames opens a wide ield o he p oduc ion o ene gy
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om was es [7]. The cooled wall eac o de eloped a Uni e si y o Valladolid is he only
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eac o p o o ype cu en ly in ope a ion wi h hyd o he mal lame as in e nal hea sou ce
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ha p oduces a educed liquid e luen wi h dissol ed solids and a high-p essu e and high-
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empe a u e e luen a 600-650 ºC and 23 MPa, ha is able o p oduce wo k and he mal
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ene gy in a mo e e icien way ha he below igni ion ubula eac o s e luen [8].
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E en when he op ion o di ec expansion o he e luen is, by a , he mos
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ene ge ically e icien , i will be no applicable in he sho e m. This is mainly due o he
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ac ha he composi ion o he e luen (50-80% mole o wa e , ca bon dioxide and
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ni ogen i ai is used as oxidan ) makes i no sui able o expansion in a con en ional
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u bine. This composi ion makes he e luen one o in e media e cha ac e is ics be ween
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he pu e wa e used in s eam u bine and he lue gases, p oduc s o combus ion used in
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gas u bines. The s a ing condi ions o his mix u e, a ound 600 ºC and 23 MPa,
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de e mine he nea -isen opic pa h needed o an e icien expansion and ou e i down
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his pa h o an ea ly condensa ion in e ms o a ull ha nessing o he mix u e en halpy
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con en ; depending on cou se on he speci ic composi ion o he mix u e. Thus, echnical
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issues conce ning he expansion o wo-phase s eams p e en he e ec i e
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implemen a ion o di ec expansion in he sho e m. Fu he mo e, he de ailed design o
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a dedica ed, e ec i e u bine would be cos ly and would ake a long ime o be ca ied
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ou . Mo eo e , he design o such a u bine would be highly dependen on he mass low
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a e o he e luen s eam, no allowing o wide a ia ion wi hou loss o e iciency.
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The e o e, a comme cial gas u bine is p oposed, whe e he eac o ou le s eam is
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injec ed in o a e he combus o . Be o e he injec ion, his s eam is mixed wi h he
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combus ion gases, his me hod allows he ene gy eco e y using a con en ional
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equipmen (expande u bine sec ion) because his doesn’ change in excess he
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expanding lue gases s eam p ope ies.
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2. Ma e ial and me hods
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2.1. Pilo Plan desc ip ion
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The simpli ied PFD (P ocess Flow Diag am) o he cooled wall eac o acili y placed
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a Uni e sidad de Valladolid is shown in Figu e 1. The plan can be used o oxidize
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a ious compounds wi h ai as oxidan in an aqueous en i onmen . The maximum
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ope a ing p essu e is 30 MPa a empe a u es be ween 400°C and 700°C wi h a maximum
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ea men capaci y o 25 kg/h o eed.
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The main equipmen o his pilo plan is he eac o . This de ice has h ee inle lines
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and wo ou le lines [8]: he eed line, en e ing a he bo om o he eac o essel and
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p oceeding down-up inside o a ubula injec o o he op o he eac o , consis o a
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pumpable mix u e o wa e and uel which is p essu ized and p ehea ed elec ically; ai
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line is in oduced a he bo om o he eac o a e comp ession, hea ing and mixing wi h
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he eed; and he hi d inle line consis s o an auxilia y downwa d low o wa e a he
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op o he eac o in ended o p o ec he eac o wall om high empe a u e. The liquid
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p oduc s line lea es he eac o om he bo om and is mainly composed o wa e and
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sal s; and he apo line lows om he op o he eac o and is mainly composed o wa e
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apo , ni ogen and ca bon dioxide wi h composi ion depending on he na u e o he uel
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was e. The ou le lines a e cooled and dep essu ized.
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The eac ion chambe consis s o a e ical ube. I is su ounded and con ained in a
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p essu e essel. Be ween he p essu e essel and he eac ion chambe he down low o
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cooling wa e keeping he empe a u e o he p essu e s anding wall unde 400°C. The
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eed is p emixed wi h ai and en e s he eac ion chambe h ough a ubula injec ion lance
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[9]. Usually he hyd o he mal lame is p oduced abo e he lance, a he op o he eac ion
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chambe , whe e he maximum empe a u e is de ec ed [9]. To p ehea he eac o a he
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s a up o he p ocess he e a e wo elec ical hea e s. The oom empe a u e cooling
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wa e en e s a he op end o he eac o lowing down be ween he walls o he eac ion
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chambe and p essu e essel. A he bo om end i o ms a pool o liquid wa e whe e i
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mixes wi h he eac ion p oduc s and can sol e sal s o a oid la ge sal deposi s inside he
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eac ion chambe .
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Da a om his acili y a e used as he base o his wo k [8].
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2.2. Ene gy In eg a ion
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As s a ed abo e, he use o supe c i ical wa e as eac ion media equi es ex eme
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p essu e and empe a u e ope a ional condi ions en ailing high-ene gy ope a ional
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expendi u e. Liquid wa e can be comp essed using a pump wi h a o dable ene gy cos s.
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The use o supe c i ical luids makes necessa y o supply hea o high quali y (≈ 400ºC).
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Because o his, i is necessa y o s udy easonable solu ions which a e able o sol e his
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pa o he p ocess wi h a iable e iciency. One solu ion could be he in eg a ion o
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supe c i ical p ocesses wi h ene gy p oduc ion in cogene a ion o Combined Hea and
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Powe (CHP) cycles. Cogene a ion is de ined as he simul aneous p oduc ion o a ious
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o ms o ene gy –being he mos equen hea and sha wo k, i.e., powe – om one
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powe sou ce. The implemen a ion o CHP p ocesses is o en joined o he use o gas
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u bines (GT). Nowadays, he mos ex ended uel used in gas u bines is na u al gas. This
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kind o in e nal combus ion u bines own se e al ad an ages o e s eam u bines and
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diesel engines, such as, highe yields, be e lexibili y and highe e iciency [10].
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Besides, i is a compac engine, wi h lowe manpowe ope a ing needs and eady
140
a ailabili y [11]. Also, he gas u bine engine is u he ecognized o i s be e
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en i onmen al pe o mance mani es ed in cu bing o ai pollu ion and educing he
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g eenhouse e ec [12]. Fo all hese ad an ages i is p o ed ha o e he las wo decades,
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GT has seen emendous de elopmen and ma ke expansion. Gas u bines ep esen ing
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only wen y pe cen o he powe gene a ion ma ke wen y yea s ago, hey now claim
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app oxima ely o y pe cen o new capaci y addi ions [13].
146
The SCWO p ocess p oduces a high p essu e eac o ou le s eam, being hese mainly
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composed o wa e , ni ogen and ca bon dioxide and can be he mally in eg a ed i he e
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is a necessi y o hea in o he pa s o he p ocess. I he e a e no o he hea equi emen s,
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i is possible o use he excess hea o implemen a s eam injec ion in he gas u bine,
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which will imp o e he e iciency o he global p ocess. This mechanism links he p ocess
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o SCWO wi h he cogene a ion p ocess. S eam injec ion is a echnique which can
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inc ease he abili y o a plan o gene a e ex a powe wi hou bu ning ex a uel and
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equi ing mode a e capi al in es men . Fu he mo e a dec ease in NOx emissions om
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he gas u bine is p oduced and also he elec ic gene a ion e iciency o he simple and
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egene a i e cycles is imp o ed [14]. S eam Injec ed Gas Tu bines (STIG) sys ems
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ope a e as an enhancemen o he B ay on cycle. High quali y s eam is used o inc ease
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he powe ou pu and imp o e ope a ing e iciency o he basic B ay on cycle. The
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de ini e place a which his s eam is injec ed di e s acco ding o he design o he
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pa icula gas u bine; howe e mainly, high p essu e s eam is injec ed in o he high-
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p essu e sec ions o he gas u bine ia he combus o uel nozzles [11]. In i s mos basic
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o m, s eam injec ion wo ks by inc easing he global mass low a e h ough he gas
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u bine wi hou inc easing he mass o ai o be comp essed. This inc ease in he expanded
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mass low gene a es an inc ease in he o a ional o que and powe ou pu . S eam injec ion
164
echnology o e s a clea imp o emen o e he B ay on cycle while p o iding a ully
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lexible ope a ing cycle [15].
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One o he key pa ame e s ha mus be conside ed o he design o a SCWO sys em
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o ene gy p oduc ion is he choice o he oxidan . F om he eac ion poin o iew, using
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ai o oxygen shows no in luence on he con e sion o he eed oxidized [16]. Ai is he
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cheapes ma e ial, bu i con ains a la ge amoun o ni ogen ha has o be p essu ized,
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and ha ac s as a diluen ha educes he empe a u e o e luen s and, he e o e, i s
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he mal quali y. On he o he hand, c yogenic liquid oxygen ca ies no diluen s, and ai
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comp esso s could be eplaced by low consump ion c yogenic pumps. Fu he mo e, pu e
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oxygen does no need o be p ehea ed up o eed injec ion empe a u e. Howe e , he cos
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and ene gy consump ion o p oducing pu e oxygen could a ec he iabili y o he
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p ocess. An in e media e op ion is he use o oxygen-en iched ai [4].
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2.3. Analyzed schemes and me hods
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In his esea ch, di e en possibili ies o ene gy eco e y om he uppe s eam o
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he SCWO cooled wall eac o a e explo ed. This s eam is gaseous and mainly composed
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o wa e , ni ogen and ca bon dioxide. Ene ge ic e iciencies a e s udied and compa ed
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using a simula ion so wa e. Also, he mass and ene gy balances a e calcula ed o he
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p oposed schemes.
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Fo ca ying ou hese s udies, Aspen Plus V8.0 so wa e is used. This so wa e can
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be used o a wide a ie y o simula ion chemical enginee ing asks, om pa allel p ocess
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moni o ing o ope a ion modes explo a ion o g ass oo design. The app oach adop ed in
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his wo k is o de elop an Aspen simula ion low-shee ha alida es agains expe imen al
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uns o he pilo plan and hen apply his lowshee o explo e di e en p ocess se ups
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o he eco e y o ene gy om he op eac o e luen . In o de o model he
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he modynamic beha io o he mix u es he Peng-Robinson he mo package wi h
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Bos on-Ma hias (PRBM) modi ica ions was used.
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The ini ial alues used in his simula ion a e expe imen al da a which we e ob ained
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om he pilo plan e e ed abo e.
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The eed consis s o solu ions o lac ose in wa e (mass ac ion: 87% H2O and 13%
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C12H22O11) a oom condi ions (20ºC and 1 ba ) wi h a mass low a e o 13.5 kg/h. The
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mass low a e o cooling wa e necessa y is 5.6 kg/h a 20ºC and 1 ba .
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In o he eac o he nex eac ion happens:
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𝐶12𝐻22𝑂11 +12𝑂2 → 12𝐶𝑂2+11𝐻2𝑂
197
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Di e en inal al e expansion p essu es can ha e a signi ican in luence in sha
340
wo k eco e y, bu his is di icul o assess due o s ong dependencies o he maximum
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allowable alue o his p essu e on he speci ic equipmen (GT) and injec ion de ails.
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Case 0 is he mos basic con igu a ion, he e isn’ gas injec ion, and being o his
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eason he ne wo k p oduced he lowes . Wi h his con igu a ion, hea in eg a ion is
344
achie ed o jus p ehea inle s eam. Ene gy in eg a ion is imp o ed wi h gas injec ion in
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case 1.
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In case 2, 3 and 4 he high p essu e is used o inc ease ene gy p oduc ion using an
347
ejec o . The simula ion so wa e employed doesn' include an ejec o o je -s eam uni ,
348
and o his eason a simpli ied con igu a ion was used.
349
I in e media e p essu e is high, he ne wo k is highe , he e o e, case 4 is be e han
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case 2 and case 3. These cases a e imp o ed whi he case 5. All he ou le p essu e eac o
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is used o he ejec o .
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And inally, he e iciencies ob ained (Table 7) in e e y cases a e o e 25 % and going
353
o up 34.6 % in case 5.
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Acknowledgemen s
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Y.G.R. & A.M. hanks o MS3 o PhD inancial suppo . M.D.B. hanks
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MINECO o RyC ellowship (RYC-2013-13976) & MINECO p ojec CTQ2013-
357
44143-R o inancial suppo .
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Re e ences
359
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(2006) 3933-3951.
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381
Sludge des uc ion by means o a hyd o he mal lame. Op imiza ion o ammonia des uc ion
382
condi ions, Chemical Enginee ing Jou nal, 232 (2013) 1-9.
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[10] M.E. McKay, A. Rabl, A case s udy on cogene a ion, Ene gy, 10 (1985) 707-720.
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Global gas u bine news, 1996.
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399
400
401
402
403
404
405
406
407
408
409
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Tables
410
Table 1
411
Tempe a u e
(ºC)
P essu e
(ba )
Mass low
(kg/h)
Pa ial mola low
(kmol/h)
Feed
20
1
13.5
0.005 C12H22O11
0.652 H2O
Ai Reac o
20
1
10
0.073 O2
0.274 N2
Reac o Inle
(Feed and Ai
Reac o )
400
230
23.5
0.073 O2
0.274 N2
0.005 C12H22O11
0.652 H2O
Cooling Wa e
35.4
230
5.6
0.311 H2O
Lowe Reac o
Ou le
700
230
9.469
0.526 H2O
Uppe Reac o
Ou le
700
230
19.631
0.011 O2
0.274 N2
0.062 CO2
0.494 H2O
Ai Tu bine
20
1
80.9
0.589 O2
2.215 N2
Na u al Gas
20
15.6
1.349
0.003 CO2
0.076 CH4
Gas Tu bine Flue
Gases
583.8
1
82.249
0.438 O2
2.215 N2
0.079 CO2
0.151 H2O
Cooled Gas
Tu bine Gases
192
1
82.249
0.438 O2
2.215 N2
0.079 CO2
0.151 H2O
412
413
20
Table 2
414
Tempe a u e
(ºC)
P essu e
(ba )
Mass low
(kg/h)
Pa ial mola low
(kmol/h)
Injec ed S eam
676.1
15.6
19.631
0.011 O2
0.274 N2
0.062 CO2
0.494 H2O
Gas Tu bine Flue Gases
539.9
1
101.889
0.449 O2
2.489 N2
0.140 CO2
0.645 H2O
Cooled Gas Tu bine
Flue Gases
235.7
1
101.889
0.449 O2
2.489 N2
0.140 CO2
0.645 H2O
415
416
21
Table 3
417
Tempe a u e
(ºC)
P essu e
(ba )
Mass low
(kg/h)
Pa ial mola low
(kmol/h)
Ejec o Inle (Val e
Ou le )
680.7
50
19.631
0.011 O2
0.274 N2
0.062 CO2
0.494 H2O
Ai Comp esso Tu bine
20
1
77.552
0.565 O2
2.123 N2
Ai Ejec o
20
1
3.358
0.024 O2
0.092 N2
Ejec o Ou le
611.1
15.6
22.989
0.036 O2
0.366 N2
0.062 CO2
0.494 H2O
Gas Tu bine Flue Gases
523.3
1
101.889
0.449 O2
2.489 N2
0.140 CO2
0.645 H2O
Cooled Gas Tu bine
Flue Gases
227.5
1
101.889
0.449 O2
2.489 N2
0.140 CO2
0.645 H2O
418
419

22
Table 4
420
Tempe a u e
(ºC)
P essu e
(ba )
Mass low
(kg/h)
Pa ial mola low
(kmol/h)
Ejec o Inle (Val e
Ou le )
686.8
100
19.631
0.011 O2
0.274 N2
0.062 CO2
0.494 H2O
Ai Comp esso Tu bine
20
1
75.929
0.553 O2
2.079 N2
Ai Ejec o
20
1
4.981
0.036 O2
0.136 N2
Ejec o Ou le
584.1
15.6
24.612
0.048 O2
0.410 N2
0.062 CO2
0.494 H2O
Gas Tu bine Flue Gases
519.6
1
101.889
0.449 O2
2.489 N2
0.140 CO2
0.645 H2O
Cooled Gas Tu bine
Flue Gases
223.5
1
101.889
0.449 O2
2.489 N2
0.140 CO2
0.645 H2O
421
422
23
Table 5
423
Tempe a u e
(ºC)
P essu e
(ba )
Mass low
(kg/h)
Pa ial mola low
(kmol/h)
Ejec o Inle (Val e
Ou le )
692.3
150
19.631
0.011 O2
0.274 N2
0.062 CO2
0.494 H2O
Ai Comp esso Tu bine
20
1
75.089
0.547 O2
2.056 N2
Ai Ejec o
20
1
5.821
0.042 O2
0.159 N2
Ejec o Ou le
571
15.6
25.451
0.054 O2
0.433 N2
0.062 CO2
0.494 H2O
Gas Tu bine Flue Gases
517.6
1
101.889
0.449 O2
2.489 N2
0.140 CO2
0.645 H2O
Cooled Gas Tu bine
Flue Gases
221.5
1
101.889
0.449 O2
2.489 N2
0.140 CO2
0.645 H2O
424
425
426
427
428
429
430
431
432
433
434
435
436
24
Table 6
437
Tempe a u e
(ºC)
P essu e
(ba )
Mass low
(kg/h)
Pa ial mola low
(kmol/h)
Ai Comp esso Tu bine
20
1
74.290
0.541 O2
2.034 N2
Ai Ejec o
20
1
6.620
0.048 O2
0.181 N2
Ejec o Ou le
559.1
15.6
26.251
0.059 O2
0.455 N2
0.062 CO2
0.494 H2O
Gas Tu bine Flue Gases
515.8
1
101.889
0.449 O2
2.489 N2
0.140 CO2
0.645 H2O
Cooled Gas Tu bine
Flue Gases
219.5
1
101.889
0.449 O2
2.489 N2
0.140 CO2
0.645 H2O
438
439
440
441
442
443
444
445
446
447
448
449
450
451
452
25
Table 7
453
Case 0
Case 1
Case 2
Case 3
Case 4
Case 5
Ejec o Inle P essu e (ba )
-
-
50
100
150
230
Ai Ejec o (mass ac ion)
(%)
-
-
4.150
6.156
7.194
8.183
Ou le combus o
empe a u e (ºC)
1041.4
950.1
939.3
934.1
931.4
928.8
Gas Tu bine Flue Gases
Tempe a u e (ºC)
583.8
530.9
523.3
519.6
517.6
515.8
Cooled Gas Tu bine Flue
Gases Tempe a u e (ºC)
192
235.7
227.5
223.5
221.1
219.5
Ene gy consump ion by
comp esso - u bine (kW)
9.874
9.873
9.463
9.265
9.163
9.065
Ene gy p oduc ion by u bine
(kW)
12.674
15.333
15.189
15.120
15.084
15.050
Ene gy consump ion by eed
pump (kW)
0.330
0.330
0.330
0.330
0.330
0.330
Ene gy consump ion by
cooling wa e pump (kW)
0.142
0.142
0.142
0.142
0.142
0.142
Ene gy consump ion by ai
comp esso
2.328
2.328
2.328
2.328
2.328
2.328
Ne wo k (kW)
0
2.660
2.926
3.055
3.121
3.185
Ne wo k om u bine (kW)
2.800
5.460
5.726
5.855
5.921
5.985
Imp o emen pe cen age
wi h espec o case 0 (%)
95
104.5
109.107
111.464
113.75
Imp o emen pe cen age
wi h espec o p e ious case
(%)
95
4.872
2.253
1.127
1.081
E iciency (%)
0
28.934
31.828
33.231
33.949
34.645
454