Simple mechanisms of CH4 reforming with CO2 and H2O on a supported Ni/ZrO2 catalyst

Hui Yang; Hui Wang; Lisha Wei; Yong Yang; Yong-Wang Li; Xiao-Dong Wen; Haijun Jiao

doi:10.1039/d1cp04048k

Simple mechanisms of CH₄ reforming with CO₂ and H₂O on a supported Ni/ZrO₂ catalyst

Phys Chem Chem Phys. 2021 Dec 1;23(46):26392-26400. doi: 10.1039/d1cp04048k.

Authors

Hui Yang^{1

2

3}, Hui Wang^{1

2

3}, Lisha Wei^{1

2

3}, Yong Yang^{1

2}, Yong-Wang Li^{1

2}, Xiao-Dong Wen^{1

2}, Haijun Jiao⁴

Affiliations

¹ State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 030001, China. wxd@sxicc.ac.cn.
² National Energy Center for Coal to Liquids, Synfuels China Co., Ltd, Huairou District, Beijing, 101400, China.
³ University of Chinese Academy of Sciences, No. 19A Yuquan Road, Beijing, 100049, China.
⁴ Leibniz-Institut für Katalyse e. V., Albert-Einstein-Str. 29a, Rostock, 18059, Germany.

PMID: 34792065
DOI: 10.1039/d1cp04048k

Abstract

To understand the metal-support interaction of oxide supported transition metal catalysts, we computed the reaction mechanisms of dry and steam reforming of methane on a tetragonal ZrO₂(101) supported Ni catalyst. Based on the limited number of active sites on the surface, an irregular and non-ideal Ni₁₃ cluster on ZrO₂(101) is identified as a catalyst. A simple reaction mechanism is proposed, and the first direct dissociation step of CO₂, CH₄ and H₂O is the most difficult based on the computed Gibbs free energies and no surface CH_XO and CH_XOH intermediates are involved, different from that on the flat Ni(111) surface. Analysis of other supported nickel catalysts shows that not only the support but also the size and shape of the metal clusters play an important role in the reaction mechanisms and kinetics.