文献类型：期刊文献

英文题名：High-Throughput screening of metal nitrides for electrochemical nitrogen reduction

作者：Lou, Zhenxin[1];Zhou, Shuhao[2,3];Hou, Yu[1];Yang, Hua Gui[1];Yuan, Haiyang[1];Wang, Haifeng[2,3]

机构：[1]East China Univ Sci & Technol, Key Lab Ultrafine Mat, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn,Minist Educ, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Key Lab Adv Mat, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Ctr Computat Chem, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China

年份：2024

卷号：665

外文期刊名：APPLIED SURFACE SCIENCE

收录：;EI(收录号：20242116137726);WOS:【SCI-EXPANDED(收录号:WOS:001245824800001)】；

基金：This project was supported by National Key R & D Program of China (2021YFA1500700) , National Natural Science Foundation of China (92045303, 51972111, 22379043) , Science and Technology Commis- sion of Shanghai Municipality (23ZR1416800) , National Ten Thousand Talent Program for Young Top-notch Talent, "Dawn" Program of Shanghai Education Commission (22SG28) , Innovation Program of Shanghai Municipal Education Commission (E00014) and Fundamental Research Funds for the Central Universities (JKD01231632) .

语种：英文

外文关键词：High -throughput screening; Density functional theory; Automated workflow; Nitrogen reduction reaction; Metal nitrides

摘要：Metal nitrides have garnered considerable attention in the context of nitrogen reduction reactions (NRR) due to their rich lattice nitrogen and abundant nitrogen vacancies to activate N2. However, the identification of suitable metal nitrides with superior stability, activity, and selectivity (vs. hydrogen evolution reaction, HER) for electrochemical NRR under rigorous isotope labeling experiments remains a perplexing challenge in experiments. In this study, we implemented a systematic screening protocol to assess the electrochemical stability and efficiency of various metal nitrides for NRR by high-throughput density functional theory calculations, aiming to search out promising metal nitride catalysts. Through a set of predetermined criteria, a subset of 6 candidates emerges as the most promising metal nitrides for NRR from a pool of 668 metal nitrides sourced from the Materials Project Database, all of which catalyze NRR following the Mars-van Krevelen pathway. Importantly, based on the analysis of these candidates, the unique structural property (i.e., four(or three)-coordinate lattice nitrogen) and energy descriptor (i.e., the formation energy of the lattice nitrogen vacancy is around 2.1 eV) of potential metal nitrides for electrochemical NRR were extracted, which could be used as the direction to rationally design metal nitride catalyst. This research not only serves as a valuable guide for experimental investigations into potential metal nitrides for NRR, but also provides an efficient method for high-throughput screening of potential catalysts for other electrochemical reactions.