Valence electron matching law for MXene-based single-atom catalysts  

作　　者：Pei Song Yuhang Zhou Zishan Luo Hang Zhang Xi Sun Sen Lu Zepeng Jia Hong Cui Weizhi Tian Rong Feng Lingxia Jin Hongkuan Yuan 

机构地区：[1]School of Mechanical Engineering,Shaanxi University of Technology,Hanzhong 723001,Shaanxi,China [2]Shaanxi Key Laboratory of Industrial Automation,Shaanxi University of Technology,Hanzhong 723001,Shaanxi,China [3]Shaanxi Key Laboratoy of Catalyis,College of Chemical Environment Science,Shaanxi Universty of Technoogy Hanzhong 723001,Shaanx,China [4]School of Physical Science and Technology,Southwest University,Chongqing 400715,China

出　　处：《Journal of Energy Chemistry》2025年第2期641-650,I0013,共11页能源化学(英文版)

基　　金：funded by the National Natural Science Foundation of China(61701288,51706128);the Natural Science Basic Research Program of Shaanxi Province(2021JM-485);the Key Scientific Research Project of Shaanxi Provincial Education Department(20JS019);the High-level Achievement Cultivation Project of Collaborative Innovation Center for Comprehensive Development of Qinba Biological Resources(QBXT-17-8);the Postgraduate Innovation Project of Shaanxi University of Technology(SLGYCX2410).

摘　　要：Single-atom catalysts(SACs)have attracted considerable interest in the fields of energy and environmental science due to their adjustable catalytic activity.In this study,we investigated the matching of valence electron numbers between single atoms and adsorbed intermediates(O,N,C,and H)in MXene-anchored SACs(M-Ti_(2)C/M-Ti_(2)CO_(2)).The density functional theory results demonstrated that the sum of the valence electron number(VM)of the interface-doped metal and the valence electron number(VA)of the adsorbed intermediates in M-Ti_(2)C followed the 10-valence electron matching law.Furthermore,based on the 10-valence electron matching law,we deduced that the sum of the valence electron number(k)and VMfor the molecular adsorption intermediate interactions in M-Ti_(2)CO_(2)adhered to the 11-valence electron matching law.Electrostatic repulsion between the interface electrons in M-Ti_(2)CO_(2)and H_(2)O weakened the adsorption of intermediates,Furthermore,we applied the 11-valence electron matching law to guide the design of catalysts for nitrogen reduction reaction,specifically for N_(2)→NNH conversion,in the MTi_(2)CO_(2)structure.The sure independence screening and sparsifying operator algorithm was used to fit a simple three-dimensional descriptor of the adsorbate(R_(2)up to 0.970)for catalyst design.Our study introduced a valence electron matching principle between doped metals(single atoms)and adsorbed intermediates(atomic and molecular)for MXene-based catalysts,providing new insights into the design of high-performance SACs.

关 键 词：Density functional theory Nitrogen reduction reaction Sure independence screening and sparsifying operator Valence electron matching law 

分 类 号：O64[理学—物理化学]