文献类型：期刊文献

英文题名：Identifying Activity Trends for the Electrochemical Production of H2O2 on M-N-C Single-Atom Catalysts Using Theoretical Kinetic Computations

作者：Shen, Jianhua[1];Wen, Yingqiang[1];Jiang, Haibo[1];Yu, Shengwei[1];Dong, Chunxiao[1];Fan, Yu[2];Liu, Bin[3];Li, Chunzhong[2]

机构：[1]East China Univ Sci & Technol, Sch Mat Sci & Engn, Frontiers Sci Ctr Materiobiol & Dynam Chem, Minist Educ,Key Lab Ultrafine Mat,Shanghai Engn R, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, Shanghai Engn Res Ctr Hierarch Nanomat, Shanghai 200237, Peoples R China;[3]Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China

年份：2022

卷号：126

期号：25

起止页码：10388

外文期刊名：JOURNAL OF PHYSICAL CHEMISTRY C

收录：;EI(收录号：20223012421996);WOS:【SCI-EXPANDED(收录号:WOS:000819929900001)】；

基金：This work was supported by the National Natural Science Foundation of China (22178106 and 21978087) , the Shanghai Scienti fi c and Technological Innovation Project (19JC1410400) , the Innovation Program of Shanghai Municipal Education Commission, the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutes of High Learning, and the Fundamental Research Funds for the Central Universities (222201718002) .

语种：英文

外文关键词：Desorption - Electrolytes - Electrolytic reduction - Iron compounds - Kinetics - Manganese compounds - Nickel compounds - Oxygen - Reaction intermediates

摘要：catalysts (SACs) have shown high potential to generate H2O2 through the two-electron oxygen reduction reaction (2e??? ORR) pathway in an acidic electrolyte. However, there is still a lack of effective kinetic computation to reveal M???N???C SACs??? intrinsic catalytical performance toward 2e??? ORR. Here, we combine the experimental and computational efforts to study the 2e??? ORR activity trends of M???N???C SACs (M = Co, Fe, and Mn). The experimental results show that Co???N???C and Mn???N???C SACs favor the 2e??? ORR pathway but Fe???N???C SAC favors the 4e??? ORR pathway. Using systematic kinetic calculation, we demonstrated that desorption of HOOH* or H2O* was a real determining step of the ORR pathway on M???N???C SACs. The difference in the desorption energy between H2O* and HOOH* reaction oxygen intermediates (EH2O* ??? EHOOH*) on a metal active center is a credible descriptor to illustrate and predict the H2O2 selectivity of M???N???C SACs. The predicted high H2O2 selectivity of Ni???N???C SACs from the descriptor is consistent with the experimental results. This study clarifies the mechanism of ORR on M???N???C SACs and identifies the determining factors of the ORR pathway, providing new insights into the rational design of high-H2O2-selectivity M???N???C SACs.