文献类型：期刊文献

英文题名：Boosting the oxygen reduction reaction behaviour of atomic Fe-N4 active sites in porous honeycomb-like carbon via P heteroatom doping

作者：Li, Jin[1];Fan, Kaicai[2];Jiang, Hongliang[3];Lu, Fenghong[1];Cui, Lixiu[1];Li, Bin[2];Zhang, Qi[1];Fan, Gao-Chao[1];Zong, Lingbo[1];Wang, Lei[1,4]

机构：[1]Qingdao Univ Sci & Technol, Coll Chem & Mol Engn, Key Lab Ecochem Engn, Qingdao 266042, Peoples R China;[2]Qingdao Univ Sci & Technol, Coll Mat Sci & Engn, Qingdao 266042, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem Engn, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China;[4]Qingdao Univ Sci & Technol, Coll Environm & Safety Engn, Shandong Engn Res Ctr Marine Environm Corros & Sa, Qingdao 266042, Peoples R China

年份：2022

卷号：10

期号：35

起止页码：18147

外文期刊名：JOURNAL OF MATERIALS CHEMISTRY A

收录：;EI(收录号：20223512668934);WOS:【SCI-EXPANDED(收录号:WOS:000842224700001)】；

基金：This work was supported financially by the National Natural Science Foundation of China, China (grant no. 52172208, 52072197, 21971132, 22074073), Natural Science Foundation of Shandong Province, China (ZR2019MB042), Outstanding Youth Foundation of Shandong Province, China (ZR2019JQ14), Youth Innovation and Technology Foundation of Shandong Higher Education Institutions, China (2019KJC004), Major Scientific and Technological Innovation Project (2019JZZY020405), Major Basic Research Program of Natural Science Foundation of Shandong Province under grant (ZR2020ZD09), and Taishan Scholar Young Talent Program (tsqn201909114). This research was undertaken on the X-ray absorption spectroscopy (XAS) at Shanghai Synchrotron Radiation Facility.

语种：英文

外文关键词：Atoms - Carbon - Catalyst activity - Electrolysis - Electrolytic reduction - Free energy - Honeycomb structures - Iron compounds - Metal working - Oxygen

摘要：Fe-N-C single atom electrocatalysts (SAECs) with porphyrin-like Fe-N-4 species are one of the most promising alternatives to the platinum-group-metal-based electrocatalysts used for oxygen reduction reaction (ORR). However, limited attention is paid on delicately optimizing the free energy barrier of Fe-N-4 active sites through heteroatom doping in the carbon skeleton. Herein, Fe single atoms (SAs) on heteroatoms N- and P-codoped porous honeycomb-like carbon (Fe-N-4/NP-PHC) have been rationally designed. The as-developed Fe-N-4/NP-PHC catalyst with abundant accessible active sites showed an impressive onset potential (E-onset = 1.0 V) and half-wave potential (E-1/2 = 0.89 V) under low electrocatalyst loading capacity, which is more positive than those of Pt/C and most SAECs. Encouragingly, the experimental results and DFT calculations systematically demonstrated that the optimized adsorption energy of the Fe-N-4 sites in the P-doped carbon matrix facilitated the release of OH* and thus boosted the ORR performance. The metal-air battery containing Fe-N-4/NP-PHC exhibited high peak power density and long-term working feasibility with a low voltage gap at large current densities. This study demonstrates that P doping in carbon matrix is an effective strategy to promote catalytic properties and presents a novel avenue for developing high-performance electrocatalysts for various electrochemical reactions.