文献类型：期刊文献

英文题名：Towards the object-oriented design of active hydrogen evolution catalysts on single-atom alloys

作者：Zhou, Chuan[1];Zhao, Jia Yue[2];Liu, Peng Fei[2];Chen, Jianfu[1];Dai, Sheng[3];Yang, Hua Gui[2];Hu, P.[1,4];Wang, Haifeng[1]

机构：[1]East China Univ Sci & Technol, Key Lab Adv Mat, Ctr Computat Chem, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Key Lab Ultrafine Mat, Minist Educ, Shanghai Engn Res Ctr Hierarch Nanomat, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Inst Fine Chem, Key Lab Adv Mat, Feringa Nobel Prize Scientist Joint Res Ctr, Shanghai 200237, Peoples R China;[4]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland

年份：2021

卷号：12

期号：31

起止页码：10634

外文期刊名：CHEMICAL SCIENCE

收录：;EI(收录号：20213310789654);WOS:【SCI-EXPANDED(收录号:WOS:000673617500001)】；

基金：This project was supported by the National Key R&D Program of China (2018YFA0208602), NSFC (21873028, 91945302, 21703067), National Ten Thousand Talent Program for Young Top-notch Talents in China, Shanghai ShuGuang project (17SG30), and the Fundamental Research Funds for the Central Universities. S. D. acknowledges support from the Shanghai Rising-Star Program (20QA1402400). Additional support was provided by the Feringa Nobel Prize Scientist Joint Research Center.

语种：英文

外文关键词：Nickel compounds - Aluminum alloys - Density functional theory - Genetic algorithms - Global optimization - Hydrogen - Catalysis - Catalysts - Inverse problems

摘要：Given a desired property, locating relevant materials is always highly desired but very challenging in a range of areas, including heterogeneous catalysis. Obviously, object-oriented design/screening is an ideal solution to this problem. Herein, we develop an inverse catalyst design workflow in Python (CATIDPy) that utilizes a genetic-algorithm-based global optimization method to guide on-the-fly density functional theory calculations, successfully realizing the highly accelerated location of active single-atom alloy (SAA) catalysts for the hydrogen evolution reaction (HER). 70 binary and 752 ternary SAA candidate catalysts are identified for the HER. Furthermore, via considering the segregation stability and cost of materials, we extracted 6 binary and 142 ternary SAA candidate catalysts that are recommended for experimental synthesis. Remarkably, guided by these theoretical identifications, homogeneously dispersed Ni-based bimetallic catalysts (e.g., NiMo, NiAl, Ni3Al, NiGa, and NiIn) were synthesized experimentally to test the reliability of the CATIDPy workflow, and they showed superior HER performance to bare Ni foam, indicating huge potential for use in real-world water electrolysis techniques. Perhaps more importantly, these results demonstrate the capacity of such a proposed approach for investigating unexplored chemical spaces to efficiently design promising catalysts without knowledge from the expert domain, which has far-reaching implications.