Rational design of bimetallic MXene solid solution with High-Performance electrocatalytic N2 reduction

Qiao-Jun Fang; Wei Zhang; Xian-Jie Zhang; Jia-Hao Wang; Shuang-Te Zhao; Xue-Long Zhang; Wen-Xian Chen; Gui-Lin Zhuang

doi:10.1016/j.jcis.2023.02.094

Rational design of bimetallic MXene solid solution with High-Performance electrocatalytic N₂ reduction

J Colloid Interface Sci. 2023 Jun 15:640:67-77. doi: 10.1016/j.jcis.2023.02.094. Epub 2023 Feb 20.

Authors

Qiao-Jun Fang¹, Wei Zhang¹, Xian-Jie Zhang¹, Jia-Hao Wang¹, Shuang-Te Zhao¹, Xue-Long Zhang¹, Wen-Xian Chen¹, Gui-Lin Zhuang²

Affiliations

¹ Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, P.R. China.
² Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, P.R. China. Electronic address: glzhuang@zjut.edu.cn.

PMID: 36841173
DOI: 10.1016/j.jcis.2023.02.094

Abstract

Electrocatalytic N₂ reduction reaction (eNRR) was an effective alternative method for green synthesis of NH₃. By combining the first-principal Density functional theory (DFT) calculations and Monte Carlo (MC) simulation, we systematacially investigated 24 types equal-ratio bimetallic MXene solid solution, involving 88 different catalysts. Our focus was on the catalytic performance of these materials in eNRR. The computational result indicate that MoW(3Mo) has high stability, selectivity (93.8 % against the hydrogen evolution reaction (HER)) and activity (U_L = -0.26 V), which is significantly better than that of monometal Mo₂CO₂ and W₂CO₂. This improvement in catalytic properties is attributed to the unique electronic structure (e.g. d-band center, charge) of bimetallic MXene solid solution. In explicit solvent conditions, the microenvironment of hydrogen bond in aqueous liquid thermodynamically promotes the catalytic property for eNRR and reduce the catalytic property of HER side reaction, but the kinetic barrier is also increased due to the effect of the hydrogen-bond microenvironment on proton migration. Overall, the obtained bimetallic MXene solid solution MoW(3Mo) exhibits excellent catalytic performance in eNRR.

Keywords: Density functional theory calculation; MXene solid solution; Monte Carlo simulation; N(2) Reduction.