Data-Driven Design of Single-Atom Electrocatalysts with Intrinsic Descriptors for Carbon Dioxide Reduction Reaction  

作　　者：Xiaoyun Lin Shiyu Zhen Xiaohui Wang Lyudmila V.Moskaleva Peng Zhang Zhi-Jian Zhao Jinlong Gong 

机构地区：[1]Key Laboratory for Green Chemical Technology of Ministry of Education,School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China [2]Collaborative Innovation Center of Chemical Science and Engineering(Tianjin),Tianjin 300072,China [3]School of Economics and Management,Tianjin University of Technology and Education,Tianjin 300222,China [4]Department of Chemistry,University of the Free State,P.O.Box 339,Bloemfontein 9301,South Africa [5]Haihe Laboratory of Sustainable Chemical Transformations,Tianjin 300192,China [6]National Industry-Education Platform of Energy Storage,Tianjin University,Tianjin 300350,China [7]Joint School of National University of Singapore and Tianjin University,International Campus of Tianjin University,Binhai New City,Fuzhou 350207,Fujian,China

出　　处：《Transactions of Tianjin University》2024年第5期459-469,共11页天津大学学报（英文版）

基　　金：the National Key R&D Program of China(No.2022YFE0102000);the National Natural Science Foundation of China(Nos.22121004,U22A20409,22250008,and 22108197);the Haihe Laboratory of Sustainable Chemical Transformations,the Natural Science Foundation of Tianjin City(No.21JCZXJC00060);the Program of Introducing Talents of Discipline to Universities(No.BP0618007);the XPLORER PRIZE for financial support。

摘　　要：The strategic manipulation of the interaction between a central metal atom and its coordinating environment in single-atom catalysts(SACs)is crucial for catalyzing the CO_(2)reduction reaction(CO_(2)RR).However,it remains a major challenge.While density-functional theory calculations serve as a powerful tool for catalyst screening,their time-consuming nature poses limitations.This paper presents a machine learning(ML)model based on easily accessible intrinsic descriptors to enable rapid,cost-effective,and high-throughput screening of efficient SACs in complex systems.Our ML model comprehensively captures the influences of interactions between 3 and 5d metal centers and 8 C,N-based coordination environments on CO_(2)RR activity and selectivity.We reveal the electronic origin of the different activity trends observed in early and late transition metals during coordination with N atoms.The extreme gradient boosting regression model shows optimal performance in predicting binding energy and limiting potential for both HCOOH and CO production.We confirm that the product of the electronegativity and the valence electron number of metals,the radius of metals,and the average electronegativity of neighboring coordination atoms are the critical intrinsic factors determining CO_(2)RR activity.Our developed ML models successfully predict several high-performance SACs beyond the existing database,demonstrating their potential applicability to other systems.This work provides insights into the low-cost and rational design of high-performance SACs.

关 键 词：Density functional theory Machine learning CO_(2) reduction reaction ELECTROCATALYSTS High-throughput screening 

分 类 号：TQ426[化学工程] TP181[自动化与计算机技术—控制理论与控制工程]