Rational design of MXene-based vacancy-confined single-atom catalyst for efficient oxygen evolution reaction  

作　　者：Zhongheng Fu Guangtong Hai Xia-Xia Ma Dominik Legut Yongchao Zheng Xiang Chen 

机构地区：[1]Beijing Advanced Innovation Center for Materials Genome Engineering,Institute for Advanced Materials and Technology,University of Science and Technology Beijing,Beijing 100083,China [2]Institute of Zhejiang University-Quzhou,Zhejiang University,Quzhou 324000,Zhejiang,China [3]Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology,Department of Chemical Engineering,Tsinghua University,Beijing 100084,China [4]IT4Innovations,VSB-Technical University of Ostrava,17.listopadu 2172/15,70800 Ostrava,Czech Republic [5]Department of Condensed Matter Physics,Faculty of Mathematics and Physics,Charles University,Ke Karlovu 3,12116 Prague 2,Czech Republic [6]State Key Laboratory of NBC Protection for Civilian,Institute of Chemical Defense,Beijing 102205,China

出　　处：《Journal of Energy Chemistry》2024年第11期663-669,共7页能源化学（英文版）

基　　金：National Natural Science Foundation of China (22209094, 22209093);Research Funds of Institute of Zhejiang University-Quzhou (No. IZQ2023RCZX032);USTB Mat Com of Beijing Advanced Innovation Center for Materials Genome Engineering;Ministry of Education, Youth and Sports of the Czech Republic through the e-INFRA CZ (ID:90254);project Quantum materials for applications in sustainable technologies (QM4ST), funded as project No. CZ.02.01.01 /00/22_008/0004572。

摘　　要：Two-dimensional transition metal carbides(MXenes) have been demonstrated to be promising supports for single-atom catalysts(SACs) to enable efficient oxygen evolution reaction(OER).However,the rational design of MXene-based SACs depends on an experimental trial-and-error approach.A theoretical guidance principle is highly expected for the efficient evaluation of MXene-based SACs.Herein,highthroughput screening was performed through first-principles calculations and machine learning techniques.Ti_(3)C_(2)(OH)_(x),V_(3)C_(2)(OH)_(x),Zr_(3)C_(2)(OH)_(x),Nb_(3)C_(2)(OH)_(x),Hf_(3)C_(2)(OH)_(x),Ta_(3)C_(2)(OH)_(x),and W_(3)C_(2)(OH)_(x) were screened out based on their excellent stability.Zn,Pd,Ag,Cd,Au,and Hg were proposed to be promising single atoms anchored in MXenes based on cohesive energy analysis.Hf_(3)C_(2)(OH)_(x) with a Pd single atom delivers a theoretical overpotential of 81 mV.Both moderate electron-deficient state and high covalency of metal-carbon bonds were critical features for the high OER reactivity.This principle is expected to be a promising approach to the rational design of OER catalysts for metal-air batteries,fuel cells,and other OER-based energy storage devices.

关 键 词：MXene Single-atom catalysis Oxygen evolution reaction High-throughput calculation Machine learning 

分 类 号：TQ426[化学工程]