Unraveling the prominent role of the Rh/ZrO2-interface in the water-gas shift reaction via a first principles microkinetic study
Kauppinen, M., Melander, M., Bazhenov, A., & Honkala, K. (2018). Unraveling the prominent role of the Rh/ZrO2-interface in the water-gas shift reaction via a first principles microkinetic study. ACS Catalysis, 8(12), 11633-11647. https://doi.org/10.1021/acscatal.8b02596
Published inACS Catalysis
© 2018 American Chemical Society
The industrially important water–gas-shift (WGS) reaction is a complex network of competing elementary reactions in which the catalyst is a multicomponent system consisting of distinct domains. Herein, we have combined density functional theory calculations with microkinetic modeling to explore the active phase, kinetics, and reaction mechanism of the WGS over the Rh–ZrO2 interface. We have explicitly considered the support and metal and their interface and find that the Rh–ZrO2 interface is far more active toward WGS than Rh(111) facets, which are susceptible to CO poisoning. CO2 forming on the zirconia support rapidly transforms into formate. These findings demonstrate the central role of the interface in the water–gas-shift reaction and the importance of modeling both the support and the metal in bifunctional systems.
PublisherAmerican Chemical Society
Publication in research information system
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Related funder(s)Academy of Finland
Funding program(s)Academy Project, AoF; Postdoctoral Researcher, AoF
Additional information about fundingThe work was funded by the Academy of Finland (https://www.aka.fi/en/, grant nos. 277222 to M.K., A.B., and H.K. and 307853 to M.M.) and the University of Jyväskylä. The electronic structure calculations were made possible by the computational resources provided by the CSC IT Center for Science, Espoo, Finland (https://www.csc.fi/en/). The authors thank Prof. Leon Lefferts and Dr. Yingnan Zhao for fruitful discussions. ...
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