轴向硫配位工程增强Fe-N-C催化剂性能以助力高性能质子交换膜燃料电池
Axial Sulfur-Coordination Engineering Boosting Fe-N-C Catalysts for High-Performance Proton Exchange Membrane Fuel Cells
摘要
Abstract
Fe-N-C catalysts have long suffered from kinetically sluggish oxygen reduction reaction(ORR)due to excessive adsorp-tion strength toward oxygen intermediates and low site utilization.Heteroatom doping effectively accelerates ORR reaction kinetics through electronic structure modulation of metal sites for optimal intermediate adsorption,while chemical vapor deposition(CVD)enhances the turnover frequency(TOF)of active sites.Herein,we developed an FeSNC catalyst featuring abundant FeS1N4 sites via a dual-precursor CVD strategy.Experimental and theoretical analyses revealed that S incorpora-tion disrupts the symmetric coordination of active sites,which optimizes OH* adsorption energies from 0.212 eV to 1.194 eV.Moreover,the TOF increased from 1.98 e–1·site–1·s–1 to 6.32 e–1·site–1·s–1,significantly enhancing the intrinsic activity of the cat-alyst.More notably,the hydrophilic character of S-containing species substantially improved hydrophilicity in the S-doped catalyst,thereby promoting mass transport of oxygen and proton delivery.As a result,the FeSNC catalyst exhibited an ex-tremely high half-wave potential of 0.863 V in 0.1 mol·L–1 HClO4 and achieved a peak power density of 1.2 W·cm–2 in H2-O2 PEMFCs.This work highlights the critical role of coordination engineering.关键词
氧还原反应/Fe-N-C/杂原子掺杂/电子调控/氧传质Key words
Oxygen reduction reaction/Fe-N-C/Heteroatom doping/Electronic regulation/Mass transport引用本文复制引用
林琳,万浩,葛君杰,侯秀旋,樊哲琛,尹义轩,赵纬祎,魏恺,周雨蝶,候利娜,王颖..轴向硫配位工程增强Fe-N-C催化剂性能以助力高性能质子交换膜燃料电池[J].电化学（中英文）,2026,32(3):1-11,11.基金项目
The work was supported by the National Key Research and Development program of China(2022YFB4004100),the National Natural Science Foundation of China(U22A20396),the University of Science and Technology of China,Academic Leading Talent Cultivation Program(KY2060000272),the Chi-na Postdoctoral Science Foundation(2024M753087,GZC20241623),National Natural Science Foundation of China(22373097),the Jilin Province Science and Technology Development Program(20260601015RC).Part of the computational time is supported by the High Performance and Computing Center of Jilin Province,Network and Computing Center in Chang-chun Institute of Applied Chemistry,Chinese Acade-my of Sciences.Thank the Shanghai Synchrotron Ra-diation Facility for conducting the X-ray absorption spectroscopic experiments at BL14W1 station. （2022YFB4004100）
