Accelerating the design of catalysts for CO_(2)electroreduction to HCOOH:A data-driven DFT-ML screening of dual atom catalysts  

作　　者：Huiwen Zhu Zeyu Guo Dawei Lan Shuai Liu Min Liu Jianwen Zhang Xiang Luo Jiahui Yu Tao Wu 

机构地区：[1]College of Digital Technology and Engineering,Ningbo University of Finance&Economics,Ningbo 315175,Zhejiang,China [2]Department of Chemical and Environmental Engineering,University of Nottingham Ningbo China,Ningbo 315100,Zhejiang,China [3]Key Laboratory of Carbonaceous Wastes Processing and Process Intensification Research of Zhejiang Province,University of Nottingham Ningbo ChinaNingbo 315100,Zhejiang,China [4]School of Mechatronics and Energy Engineering,NingboTech UniversityNingbo 315104,Zhejiang,China [5]Medical Science and Technology Innovation Centre,Shandong First Medical University&Shandong Academy of Medical Sciences,Jinan 250117,Shandong,China

出　　处：《Journal of Energy Chemistry》2024年第12期627-635,共9页能源化学（英文版）

基　　金：partially sponsored by the Development and Reform Commission of Ningbo Municipality(Ningbo Municipal Engineering Research Centre for Solid Carbonaceous Wastes Processing and Utilization Technologies);the National Natural Science Foundation Youth Science Fund Project(52203300),the National Natural Science Foundation of China(22308195);the Natural Science Foundation of Shandong Province(ZR2023QB237);Ningbo Science and Technologies Innovation 2025 Major Special Project(2018B10027);The Zhejiang Provincial Department of Science and Technology is acknowledged for sponsorship under its Provincial Key Laboratory Program(2020E10018);Ningbo Bureau of Science and Technology is also thanked for its support to the Key Laboratory of Clean Energy Conversion Technologies;The University of Nottingham Ningbo China provides the first author with a full scholarship。

摘　　要：Dual-atom catalysts(DACs)have emerged as potential catalysts for effective electroreduction of CO_(2)due to their high atom utilization efficiency and multiple active sites.However,the screening of DACs remains a challenge due to the large number of possible combinations,making exhaustive experimental or computational screening a daunting task.In this study,a density functional theory(DFT)-based machine learning(ML)-accelerated(DFT-ML)hybrid approach was developed to test a set of 406 dual transition metal catalysts on N-doped graphene(NG)for the electroreduction of CO_(2)to HCOOH.The results showed that the ML algorithms can successfully capture the relationship between the descriptors of the DACs(inputs)and the limiting potential for HCOOH generation(output).Of the four ML algorithms studied in this work,the feedforward neural network model achieved the highest prediction accuracy(the highest correlation coefficient(R^(2))of 0.960 and the lowest root mean square error(RMSE)of 0.319 eV on the test set)and the predicted results were verified by DFT calculations with an average absolute error of 0.14 eV.The DFT-ML approach identified Co-Co-NG and Ir-Fe-NG as the most active and stable electrocatalysts for the electrochemical reduction of CO_(2)to HCOOH.The DFT-ML hybrid approach exhibits exceptional prediction accuracy while enabling a significant reduction in screening time by an impressive 64%compared to conventional DFT-only calculations.These results demonstrate the immense potential of using ML methods to accelerate the screening and rational design of efficient catalysts for various energy and environmental applications.

关 键 词：CO_(2)electroreduction reaction Dual atom catalysts Rapid screening Density functional theory Machine learning 

分 类 号：TQ225.121[化学工程—有机化工] O643.36[理学—物理化学]