159:. The benefits of this application are two-fold: not only would the water gas shift reaction effectively reduce the concentration of carbon monoxide, but it would also increase the efficiency of the fuel cells by increasing hydrogen production. Unfortunately, current commercial catalysts that are used in industrial water gas shift processes are not compatible with fuel cell applications. With the high demand for clean fuel and the critical role of the water gas shift reaction in hydrogen fuel cells, the development of water gas shift catalysts for the application in fuel cell technology is an area of current research interest.
471:
accounts for about 90% of the total rate owing to the thermodynamic stability of adsorbed formate on the oxide support. The active site for carboxyl formation consists of a metal atom adjacent to an adsorbed hydroxyl. This ensemble is readily formed at the metal-oxide interface and explains the much higher activity of oxide-supported transition metals relative to extended metal surfaces. The turn-over-frequency for the WGSR is proportional to the equilibrium constant of hydroxyl formation, which rationalizes why reducible oxide supports (e.g. CeO
435:
as kinetically relevant during the high-temperature WGSR (> 350 °C) over the industrial iron-chromia catalyst. Historically, there has been much more controversy surrounding the mechanism at low temperatures. Recent experimental studies confirm that the associative carboxyl mechanism is the predominant low temperature pathway on metal-oxide-supported transition metal catalysts.
427:
209:
479:) and extended metal surfaces (e.g. Pt). In contrast to the active site for carboxyl formation, formate formation occurs on extended metal surfaces. The formate intermediate can be eliminated during the WGSR by using oxide-supported atomically dispersed transition metal catalysts, further confirming the kinetic dominance of the carboxyl pathway.
434:
The WGSR has been extensively studied for over a hundred years. The kinetically relevant mechanism depends on the catalyst composition and the temperature. Two mechanisms have been proposed: an associative
Langmuir–Hinshelwood mechanism and a redox mechanism. The redox mechanism is generally regarded
417:
prevents dispersion and pellet shrinkage. The LTS shift reactor operates at a range of 200–250 °C. The upper temperature limit is due to the susceptibility of copper to thermal sintering. These lower temperatures also reduce the occurrence of side reactions that are observed in the case of the
400:
Catalysts for the lower temperature WGS reaction are commonly based on copper or copper oxide loaded ceramic phases, While the most common supports include alumina or alumina with zinc oxide, other supports may include rare earth oxides, spinels or perovskites. A typical composition of a commercial
162:
Catalysts for fuel cell application would need to operate at low temperatures. Since the WGSR is slow at lower temperatures where equilibrium favors hydrogen production, WGS reactors require large amounts of catalysts, which increases their cost and size beyond practical application. The commercial
470:
There has been significant controversy surrounding the kinetically relevant intermediate during the associative mechanism. Experimental studies indicate that both intermediates contribute to the reaction rate over metal oxide supported transition metal catalysts. However, the carboxyl pathway
383:
nature of the reaction. As such, the inlet temperature is maintained at 350 °C to prevent the exit temperature from exceeding 550 °C. Industrial reactors operate at a range from atmospheric pressure to 8375 kPa (82.7 atm). The search for high performance HT WGS catalysts remains an
331:(LTS) with intersystem cooling. The initial HTS takes advantage of the high reaction rates, but results in incomplete conversion of carbon monoxide. A subsequent low temperature shift reactor lowers the carbon monoxide content to <1%. Commercial HTS catalysts are based on
302:
199:
The equilibrium of this reaction shows a significant temperature dependence and the equilibrium constant decreases with an increase in temperature, that is, higher hydrogen formation is observed at lower temperatures.
1017:
Grabow, Lars C.; Gokhale, Amit A.; Evans, Steven T.; Dumesic, James A.; Mavrikakis, Manos (2008-03-01). "Mechanism of the Water Gas Shift
Reaction on Pt: First Principles, Experiments, and Microkinetic Modeling".
897:
Coletta, Vitor C.; Gonçalves, Renato V.; Bernardi, Maria I. B.; Hanaor, Dorian A. H.; Assadi, M. Hussein N.; Marcos, Francielle C. F.; Nogueira, Francisco G. E.; Assaf, Elisabete M.; Mastelaro, Valmor R. (2021).
388:
is a key criteria for the assessment of catalytic performance in WGS reactions. To date, some of the lowest activation energy values have been found for catalysts consisting of copper nanoparticles on
155:
by increasing hydrogen production. The WGSR is considered a critical component in the reduction of carbon monoxide concentrations in cells that are susceptible to carbon monoxide poisoning such as the
167:
in its inactive state and therefore presents safety concerns for consumer applications. Developing a catalyst that can overcome these limitations is relevant to implementation of a hydrogen economy.
459:
O dissociates onto the catalyst to yield adsorbed OH and H. The dissociated water reacts with CO to form a carboxyl or formate intermediate. The intermediate subsequently dehydrogenates to yield CO
487:
The redox mechanism involves a change in the oxidation state of the catalytic material. In this mechanism, CO is oxidized by an O-atom intrinsically belonging to the catalytic material to form CO
870:
Rodriguez, J.A.; Liu, P.; Wang, X.; Wen, W.; Hanson, J.; Hrbek, J.; Pérez, M.; Evans, J. (15 May 2009). "Water-gas shift activity of Cu surfaces and Cu nanoparticles supported on metal oxides".
1296:
Barakat, Tarek; Rooke, Joanna C.; Genty, Eric; Cousin, Renaud; Siffert, Stéphane; Su, Bao-Lian (1 January 2013). "Gold catalysts in environmental remediation and water-gas shift technologies".
73:
in 1780. It was not until much later that the industrial value of this reaction was realized. Before the early 20th century, hydrogen was obtained by reacting steam under high pressure with
720:
Jansen, Daniel; van Selow, Edward; Cobden, Paul; Manzolini, Giampaolo; Macchi, Ennio; Gazzani, Matteo; Blom, Richard; Heriksen, Partow Pakdel; Beavis, Rich; Wright, Andrew (2013-01-01).
576:
In the conversion of carbon dioxide to useful materials, the water–gas shift reaction is used to produce carbon monoxide from hydrogen and carbon dioxide. This is sometimes called the
132:/CO ratio. It provides a source of hydrogen at the expense of carbon monoxide, which is important for the production of high purity hydrogen for use in ammonia synthesis.
1322:
King, A. D.; King, R. B.; Yang, D. B., "Homogeneous catalysis of the water gas shift reaction using iron pentacarbonyl", J. Am. Chem. Soc. 1980, vol. 102, pp. 1028-1032.
379:. The operation of HTS catalysts occurs within the temperature range of 310 °C to 450 °C. The temperature increases along the length of the reactor due to the
947:
Jain, Rishabh; Maric, Radenka (April 2014). "Synthesis of nano-Pt onto ceria support as catalyst for water–gas shift reaction by
Reactive Spray Deposition Technology".
217:
409:. The active catalytic species is CuO. The function of ZnO is to provide structural support as well as prevent the poisoning of copper by sulfur. The Al
1107:
Yao, Siyu; Zhang, Xiao; Zhou, Wu; Gao, Rui; Xu, Wenqian; Ye, Yifan; Lin, Lili; Wen, Xiaodong; Liu, Ping; Chen, Bingbing; Crumlin, Ethan (2017-06-22).
237:
974:
Gokhale, Amit A.; Dumesic, James A.; Mavrikakis, Manos (2008-01-01). "On the
Mechanism of Low-Temperature Water Gas Shift Reaction on Copper".
680:
135:
The water–gas shift reaction may be an undesired side reaction in processes involving water and carbon monoxide, e.g. the rhodium-based
156:
627:
184:
1062:"Heterolytic Hydrogen Activation: Understanding Support Effects in Water–Gas Shift, Hydrodeoxygenation, and CO Oxidation Catalysis"
704:
375:, 0.2% MgO (remaining percentage attributed to volatile components). The chromium acts to stabilize the iron oxide and prevents
900:"Cu-Modified SrTiO3 Perovskites Toward Enhanced Water–Gas Shift Catalysis: A Combined Experimental and Computational Study"
1422:
1412:
1178:
Nelson, Nicholas C.; Nguyen, Manh-Thuong; Glezakou, Vassiliki-Alexandra; Rousseau, Roger; Szanyi, János (October 2019).
607:
232:. Over the temperature range of 600–2000 K, the equilibrium constant for the WGSR has the following relationship:
125:
1417:
805:
Smith R J, Byron; Muruganandam
Loganthan; Murthy Shekhar Shantha (2010). "A Review of the Water Gas Shift Reaction".
229:
343:. Sulfur compounds are removed prior to the LTS reactor by a guard bed. An important limitation for the HTS is the H
212:
Temperature dependence of the free molar (Gibbs) enthalpy and equilibrium constant of the water-gas shift reaction.
1181:"Carboxyl intermediate formation via an in situ-generated metastable active site during water-gas shift catalysis"
1427:
535:
447:
O are adsorbed onto the surface of the catalyst, followed by formation of an intermediate and the desorption of H
524:
492:
1339:
Guil-López, R.; Mota, N.; Llorente, J.; Millán, E.; Pawelec, B.; Fierro, J. L. G.; Navarro, R. M. (2019).
612:
508:
1108:
216:
With increasing temperature, the reaction rate increases, but hydrogen production becomes less favorable
1352:
1123:
721:
622:
225:
1109:"Atomic-layered Au clusters on α-MoC as catalysts for the low-temperature water-gas shift reaction"
706:
Kinetics and catalysis of the water-gas-shift reaction: A Microkinetic and Graph
Theoretic Approach
443:
In 1920 Armstrong and
Hilditch first proposed the associative mechanism. In this mechanism CO and H
221:
89:
392:
support materials, with values as low as Ea = 34 kJ/mol reported relative to hydrogen generation.
1278:
1209:
1157:
1089:
929:
911:
899:
822:
784:
651:
507:
The mechanism entails nucleophilic attack of water or hydroxide on a M-CO center, generating a
495:
at the newly formed O-vacancy to yield two hydroxyls. The hydroxyls disproportionate to yield H
347:
O/CO ratio where low ratios may lead to side reactions such as the formation of metallic iron,
116:. Its most important application is in conjunction with the conversion of carbon monoxide from
81:
and hydrogen. With the development of industrial processes that required hydrogen, such as the
1388:
1370:
1270:
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1201:
1149:
1141:
1081:
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1035:
999:
991:
746:
676:
385:
320:
316:
104:
The WGSR is a highly valuable industrial reaction that is used in the manufacture of ammonia,
93:
1341:"Methanol Synthesis from CO2: A Review of the Latest Developments in Heterogeneous Catalysis"
1378:
1360:
1323:
1305:
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1131:
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983:
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136:
339:
and the LTS catalyst is a copper-based. The copper catalyst is susceptible to poisoning by
82:
117:
35:
1227:
Nelson, Nicholas C.; Chen, Linxiao; Meira, Debora; Kovarik, Libor; Szanyi, János (2020).
1356:
1127:
319:
of the reaction, the industrial scale water gas shift reaction is conducted in multiple
1383:
1340:
336:
312:
140:
70:
43:
1406:
1282:
1234:
During
Reverse Water–Gas Shift Reaction: Formation of Atomically Dispersed Palladium"
1213:
1161:
1093:
933:
590:). The term 'shift' in water–gas shift means changing the water gas composition (CO:H
418:
HTS. Noble metals such as platinum, supported on ceria, have also been used for LTS.
164:
1180:
826:
788:
767:
Ratnasamy, Chandra; Wagner, Jon P. (September 2009). "Water Gas Shift
Catalysis".
586:
is defined as a fuel gas consisting mainly of carbon monoxide (CO) and hydrogen (H
960:
883:
741:
359:
The typical composition of commercial HTS catalyst has been reported as 74.2% Fe
348:
105:
39:
17:
1197:
856:
780:
380:
332:
176:
78:
1374:
1258:
1205:
1145:
1077:
1039:
995:
750:
297:{\displaystyle K_{\mathrm {eq} }=10^{-2.4198+0.0003855T+{\frac {2180.6}{T}}}}
1136:
583:
520:
376:
152:
92:
was needed. As a resolution to this problem, the WGSR was combined with the
1392:
1274:
1250:
1153:
1003:
925:
818:
426:
384:
intensive topic of research in fields of chemistry and materials science.
545:
430:
Proposed associative and redox mechanisms of the water gas shift reaction
113:
109:
47:
1327:
1365:
1309:
555:
128:, the WGSR is one of the most important reactions used to balance the H
121:
85:
1266:
1229:
1085:
1031:
987:
208:
632:
340:
188:
916:
401:
LTS catalyst has been reported as 32-33% CuO, 34-53% ZnO, 15-33% Al
671:
Vielstich, Wolf; Lamm, Arnold; Gasteiger, Hubert A., eds. (2003).
425:
389:
207:
499:
and return the catalytic surface back to its pre-reaction state.
187:(SEWGS) in order to produce a high pressure hydrogen stream from
69:
The water gas shift reaction was discovered by
Italian physicist
617:
74:
673:
Handbook of fuel cells: fundamentals, technology, applications
124:
or other hydrocarbons in the production of hydrogen. In the
163:
LTS catalyst used in large scale industrial plants is also
843:
Newsome, David S. (1980). "The Water-Gas Shift Reaction".
88:
synthesis, a less expensive and more efficient method of
463:
and adsorbed H. Two adsorbed H atoms recombine to form H
351:, carbon deposition, and the Fischer–Tropsch reaction.
175:
The WGS reaction is used in combination with the solid
807:
International Journal of Chemical Reactor Engineering
568:
In aqueous solution, the reaction is less exergonic.
475:) are more active than irreducible supports (e.g. SiO
324:
240:
328:
1228:
1179:
296:
1060:Nelson, Nicholas C.; Szanyi, János (2020-05-15).
220:since the water gas shift reaction is moderately
143:uses less water, which suppresses this reaction.
666:
664:
662:
660:
594:) ratio. The ratio can be increased by adding CO
654:a combined experimental and computational study
838:
836:
722:"SEWGS Technology is Now Ready for Scale-up!"
8:
698:
696:
694:
692:
598:or reduced by adding steam to the reactor.
27:Reaction of carbon monoxide and water vapor
845:Catalysis Reviews: Science and Engineering
1382:
1364:
1135:
915:
740:
282:
263:
246:
245:
239:
976:Journal of the American Chemical Society
531:
157:proton-exchange membrane (PEM) fuel cell
1239:Angewandte Chemie International Edition
1230:"In Situ Dispersion of Palladium on TiO
800:
798:
709:(PhD). Worcester Polytechnic Institute.
644:
311:In order to take advantage of both the
151:The WGSR can aid in the efficiency of
1173:
1171:
1055:
1053:
1051:
1049:
7:
762:
760:
1020:The Journal of Physical Chemistry C
1298:Energy & Environmental Science
250:
247:
25:
628:Sorption enhanced water gas shift
185:sorption enhanced water gas shift
171:Sorption enhanced water gas shift
34:(WGSR) describes the reaction of
578:reverse water–gas shift reaction
355:High temperature shift catalysis
396:Low temperature shift catalysis
228:can be explained according to
1:
527:at room temperature (298 K):
491:. A water molecule undergoes
234:
226:shift in chemical equilibrium
961:10.1016/j.apcata.2014.01.053
949:Applied Catalysis A: General
904:ACS Applied Energy Materials
884:10.1016/j.cattod.2008.08.022
742:10.1016/j.egypro.2013.06.107
608:In situ resource utilization
703:Callaghan, Caitlin (2006).
1444:
1198:10.1038/s41929-019-0343-2
857:10.1080/03602458008067535
781:10.1080/01614940903048661
652:Water Gas Shift Catalysis
1078:10.1021/acscatal.0c01059
525:thermodynamic parameters
230:Le Chatelier's principle
32:water–gas shift reaction
1137:10.1126/science.aah4321
572:Reverse water–gas shift
493:dissociative adsorption
126:Fischer–Tropsch process
1251:10.1002/anie.202007576
926:10.1021/acsaem.0c02371
819:10.2202/1542-6580.2238
613:Lane hydrogen producer
509:metallacarboxylic acid
431:
325:high temperature shift
298:
213:
204:Temperature dependence
523:, with the following
439:Associative mechanism
429:
329:low temperature shift
299:
211:
96:to produce hydrogen.
623:Industrial catalysts
327:(HTS) followed by a
238:
139:. The iridium-based
94:gasification of coal
1423:Hydrogen production
1413:Inorganic reactions
1357:2019Mate...12.3902G
1328:10.1021/ja00523a020
1245:(40): 17657–17663.
1128:2017Sci...357..389Y
675:. New York: Wiley.
560:ΔS = –10.1 cal/deg
195:Reaction conditions
90:hydrogen production
1418:Chemical processes
1366:10.3390/ma12233902
1310:10.1039/c2ee22859a
503:Homogeneous models
432:
307:Practical concerns
294:
214:
1122:(6349): 389–393.
1072:(10): 5663–5671.
1032:10.1021/jp7099702
1026:(12): 4608–4617.
988:10.1021/ja0768237
769:Catalysis Reviews
682:978-0-471-49926-8
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386:Activation energy
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218:thermodynamically
16:(Redirected from
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550:ΔH = –9.84 kcal
540:ΔG = –6.82 kcal
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321:adiabatic stages
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106:hydrocarbons
103:
100:Applications
68:
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955:: 461–468.
910:: 452–461.
536:Free energy
349:methanation
83:Haber–Bosch
77:to produce
40:water vapor
1407:Categories
1304:(2): 371.
917:2104.06739
639:References
381:exothermic
367:, 10.0% Cr
333:iron oxide
222:exothermic
177:adsorption
165:pyrophoric
153:fuel cells
147:Fuel cells
79:iron oxide
1375:1996-1944
1345:Materials
1283:220118889
1259:1521-3773
1214:202729116
1206:2520-1158
1162:206651887
1146:0036-8075
1094:218798723
1040:1932-7447
996:0002-7863
934:233231670
751:1876-6102
584:Water gas
521:exergonic
422:Mechanism
377:sintering
274:0.0003855
265:−
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1275:32589820
1154:28642235
1004:18181624
827:96769998
813:: 1–32.
789:98530242
602:See also
546:Enthalpy
317:kinetics
114:hydrogen
110:methanol
48:hydrogen
42:to form
1384:6926878
1353:Bibcode
1267:1661896
1124:Bibcode
1116:Science
1086:1656557
556:Entropy
224:; this
183:in the
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86:ammonia
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451:and CO
341:sulfur
285:2180.6
268:2.4198
189:syngas
112:, and
58:O ⇌ CO
54:CO + H
1279:S2CID
1210:S2CID
1158:S2CID
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1090:S2CID
930:S2CID
912:arXiv
823:S2CID
785:S2CID
725:(PDF)
390:ceria
179:of CO
1389:PMID
1371:ISSN
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1255:ISSN
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1150:PMID
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1036:ISSN
1000:PMID
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747:ISSN
677:ISBN
618:PROX
315:and
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