A theoretical study of the reverse water‐gas shift reaction on Ni(111) and Ni(311) surfaces. (6th November 2019)

• Record Type: Journal Article
• Authors: Zhang, Min; Zijlstra, Bart; Filot, Ivo A. W.; Li, Fang; Wang, Haiou; Li, Jingde; Hensen, Emiel J. M.
• Is Part Of: Canadian journal of chemical engineering. Volume 98:Number 3(2020)
• Page Start: 740
• Page End: 748
• Publication Date: 2019-11-06
• Subjects: carbon dioxide -- DFT -- nickel -- reverse water‐gas shift -- surface redox; Chemical engineering -- Periodicals; Technology -- Periodicals; 660.05
• DOI: 10.1002/cjce.23655
• Languages: English
• ISSNs: 0008-4034

Abstract

Abstract: This paper presents a systematic comparison study of the surface redox reaction mechanism for reverse water‐gas shift (RWGS) over Ni(111) and Ni(311) surfaces. Specifically, the most stable surface intermediates and the reaction kinetics involved in the direct CO2 activation and water formation steps are computed with density functional theory calculations and compared for the two different Ni surfaces. The results show that CO2, CO, O, H, OH, and H2 O species adsorb stronger on Ni(311) than on Ni(111). Compared to Ni(111), the overall barriers for direct CO2 activation and water formation on Ni(311) are lower by 23 and 17 kJ/mol, respectively. These observations indicate that the RWGS reaction through the surface redox mechanism should be preferred on Ni(311). Abstract : Comparison of flat and stepped surfaces of Ni catalysts for surface redox mechanism of the RWGS reaction.