TY - JOUR
T1 - An active, stable cubic molybdenum carbide catalyst for the high-temperature reverse water-gas shift reaction
AU - Khoshooei, Milad Ahmadi
AU - Wang, Xijun
AU - Vitale, Gerardo
AU - Formalik, Filip
AU - Kirlikovali, Kent O.
AU - Snurr, Randall Q.
AU - Pereira-Almao, Pedro
AU - Farha, Omar K.
N1 - Publisher Copyright:
© 2024 American Association for the Advancement of Science. All rights reserved.
PY - 2024/5/3
Y1 - 2024/5/3
N2 - Although technologically promising, the reduction of carbon dioxide (CO2) to produce carbon monoxid (CO) remains economically challenging owing to the lack of an inexpensive, active, highly selective, and stable catalyst. We show that nanocrystalline cubic molybdenum carbide (a-Mo2C), prepared through a facile and scalable route, offers 100% selectivity for CO2 reduction to CO while maintaining it initial equilibrium conversion at high space velocity after more than 500 hours of exposure to harsh reaction conditions at 600°C. The combination of operando and postreaction characterization of the catalyst revealed that its high activity, selectivity, and stability are attributable to crystallographic phase purity, weak CO-Mo2C interactions, and interstitial oxygen atoms, respectively. Mechanistic studies and density functional theory (DFT) calculations provided evidence that the reaction proceeds through an H2-aided redox mechanism.
AB - Although technologically promising, the reduction of carbon dioxide (CO2) to produce carbon monoxid (CO) remains economically challenging owing to the lack of an inexpensive, active, highly selective, and stable catalyst. We show that nanocrystalline cubic molybdenum carbide (a-Mo2C), prepared through a facile and scalable route, offers 100% selectivity for CO2 reduction to CO while maintaining it initial equilibrium conversion at high space velocity after more than 500 hours of exposure to harsh reaction conditions at 600°C. The combination of operando and postreaction characterization of the catalyst revealed that its high activity, selectivity, and stability are attributable to crystallographic phase purity, weak CO-Mo2C interactions, and interstitial oxygen atoms, respectively. Mechanistic studies and density functional theory (DFT) calculations provided evidence that the reaction proceeds through an H2-aided redox mechanism.
UR - http://www.scopus.com/inward/record.url?scp=85192039730&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85192039730&partnerID=8YFLogxK
U2 - 10.1126/science.adl1260
DO - 10.1126/science.adl1260
M3 - Article
C2 - 38696554
AN - SCOPUS:85192039730
SN - 0036-8075
VL - 384
SP - 540
EP - 546
JO - Science
JF - Science
IS - 6695
ER -