Rational design of highly efficient MXene-based catalysts for the water-gas-shift reaction

Zhang, Zhe1,2; Zheng, Baobing3; Tian, Hao2,4; He, Yanling2,4; Huang, Xiang2; Ali, Sajjad2; Xu, Hu2,5,6

2022-07-01

10.1039/d1cp05789h

PHYSICAL CHEMISTRY CHEMICAL PHYSICS   Impact Factor & Quartile

1463-9076

1463-9084

Water molecules linked by hydrogen bonds are responsible for the high efficiency of bi-functional catalysts for the water-gas-shift (WGS) reaction because water can act as a proton transfer medium. Herein, we propose an associative pathway for the WGS reaction assisted by water to realize hydrogen production. Based on this pathway, we show by first-principles calculations that a large family of oxygen-terminated two-dimensional transition metal carbides and nitrides (MXenes) deposited on Au clusters are promising catalysts for the WGS reaction. Remarkably, the rate-determining barriers for *CO -> *COOH on Au/Mn+1XnO2 are in the range from 0.15 eV to 0.39 eV, indicating that WGS can occur at much lower temperatures. Furthermore, a comprehensive microkinetic model is constructed to describe the turnover frequencies (TOF) for the product under the steady-state conditions. More importantly, there is a perfect linear scaling relationship between the rate-determining barriers of the WGS and the free energy of the adsorbed hydrogen. Besides, the potential energy diagrams for CO reforming reveal that the F terminations introduced in experiments have only a slight influence on the catalytic performance of the oxygen-terminated MXenes. Our work not only opens a new avenue towards the WGS reaction but also provides many ideal catalysts for hydrogen production.

SCI ; EI

English

Corresponding

Guangdong Natural Science Funds for Distinguished Young Scholars[2017B030306008] ; National Natural Science Foundation of China[11974160] ; Science, Technology and Innovation Commission of Shenzhen Municipality["RCYX20200714114523069","ZDSYS201909020929052 85"] ; Guangdong Provincial Key Laboratory of Computational Science and Material Design[2019B030301001]

Chemistry ; Physics

Chemistry, Physical ; Physics, Atomic, Molecular & Chemical

WOS:000830472100001

ROYAL SOC CHEMISTRY

20223212532027

Calculations ; Carbides ; Catalyst activity ; Chemical shift ; Free energy ; Gibbs free energy ; Gold compounds ; Hydrogen bonds ; Hydrogen production ; Manganese compounds ; Molecules ; Transition metals ; Water gas shift

Gas Fuels:522 ; Metallurgy and Metallography:531 ; Thermodynamics:641.1 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Ceramics:812.1 ; Mathematics:921 ; Atomic and Molecular Physics:931.3

CHEMISTRY

Web of Science

1.Yangzhou Univ, Coll Phys Sci & Technol, Yangzhou 225002, Jiangsu, Peoples R China
2.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
3.Baoji Univ Arts & Sci, Coll Phys & Optoelect Technol, Nonlinear Res Inst, Baoji 721016, Peoples R China
4.Univ Hong Kong, Dept Phys, Hong Kong, Peoples R China
5.Southern Univ Sci & Technol, Guangdong Prov Key Lab Computat Sci & Mat Design, Shenzhen 518055, Peoples R China
6.Southern Univ Sci & Technol, Shenzhen Key Lab Adv Quantum Funct Mat & Devices, Shenzhen 518055, Peoples R China

Zhang, Zhe,Zheng, Baobing,Tian, Hao,et al. Rational design of highly efficient MXene-based catalysts for the water-gas-shift reaction[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2022,24:18265-18271.

Zhang, Zhe.,Zheng, Baobing.,Tian, Hao.,He, Yanling.,Huang, Xiang.,...&Xu, Hu.(2022).Rational design of highly efficient MXene-based catalysts for the water-gas-shift reaction.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,24,18265-18271.

Zhang, Zhe,et al."Rational design of highly efficient MXene-based catalysts for the water-gas-shift reaction".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 24(2022):18265-18271.