A1 Journal article (refereed)
Unraveling the prominent role of the Rh/ZrO2-interface in the water-gas shift reaction via a first principles microkinetic study (2018)

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

JYU authors or editors

Melander, Marko
Bazhenov, Andrey
Honkala, Karoliina
Kauppinen, Minttu

Publication details

All authors or editors: Kauppinen, Minttu; Melander, Marko; Bazhenov, Andrey; Honkala, Karoliina

Journal or series: ACS Catalysis

ISSN: 2155-5435

eISSN: 2155-5435

Publication year: 2018

Volume: 8

Issue number: 12

Pages range: 11633-11647

Publisher: American Chemical Society

Publication country: United States

Publication language: English

DOI: https://doi.org/10.1021/acscatal.8b02596

Publication open access: Not open

Publication channel open access:

Publication is parallel published (JYX): https://jyx.jyu.fi/handle/123456789/60267

Abstract

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.

Keywords: gases; chemical reactions; catalysis; interfaces (surfaces); interfacial phenomena; density functional theory

Free keywords: water-gas shift; heterogeneous catalysis; microkinetics; metal-support interface

Fields of science: