文献类型：期刊文献

英文题名：Regulating the Electronic Configuration of Single-Atom Catalysts with Fe-N5 Sites via Environmental Sulfur Atom Doping for an Enhanced Oxygen Reduction Reaction

作者：Yang, Kun-Zu[1];Xu, Chao[1];Guo, Peng-Peng[1];Zhao, Ye-Min[1];Chi, Hua-Min[1];Xu, Ying[1];Wei, Ping-Jie[1];Zheng, Tianlong[2];He, Qinggang[2];Ren, Qizhi[3];Liu, Jin-Gang[1]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Zhejiang, Peoples R China;[3]Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China

年份：2024

卷号：12

期号：29

起止页码：11033

外文期刊名：ACS SUSTAINABLE CHEMISTRY & ENGINEERING

收录：;EI(收录号：20242916715006);WOS:【SCI-EXPANDED(收录号:WOS:001274489700001)】；

基金：This study was financially supported by the National Natural Science Foundation of China (Nos. 21571062, 22178307), the Program for Professor of Special Appointment (Eastern Scholar) at the Shanghai Institutions of Higher Learning, and the Fundamental Research Funds for the Central Universities (No. 222201717003).

语种：英文

外文关键词：single-atom catalyst; Fe-N-5 activesite; oxygen reduction reaction; atom economy; environmental S-doping engineering

摘要：Heteroatom doping is considered an essential strategy to modulate the Fe-N-C catalytic activity for the oxygen reduction reaction (ORR) in energy conversion technologies. However, challenges remain in achieving a singular form of heteroatom doping, i.e., asymmetrical coordination with metal sites and heteroatom doping in environmental skeleton carbons. And a low doping efficiency and inappropriate doping ratios result in the excessive use of heteroatom-containing organic additives, further limiting the achievement of sustainability. In this work, we prepared an atom-economical Fe-N-5 single-atom catalyst (SAC) with only environmental S atom doping, which was synthesized by pyrolyzing an axial imidazole-coordinated thiophene iron porphyrin precursor on PVI-functionalized carbon black. Due to the electron-donating properties of thiophene-S atoms, the intrinsic activity of the Fe-N-5 site was significantly promoted by regulating the electronic configuration through the long-range interaction, thus lowering the energy barrier of the ORR. As expected, the resultant catalyst exhibited an efficient ORR activity in alkaline media and in the aqueous zinc-air battery, with a higher half-wave potential of 0.89 V vs RHE and a maximum power density of 147 mW cm(-2) than those of 20 wt % Pt/C (E-1/2 = 0.87 V, P-max = 120 mW cm(-2)). This work provides a facile heteroatom-doping engineering approach to boost the intrinsic catalytic activity of advanced SACs in energy conversion applications.