Amino-metalloporphyrin polymers derived Fe single atom catalysts for highly efficient oxygen reduction reaction  

作　　者：Qian He Yuying Meng Hao Zhang Ying Zhang Qingdi Sun Tao Gan Huajian Xiao Xiaohui He Hongbing Ji 

机构地区：[1]Fine Chemical Industry Research Institute,School of Chemistry,Sun Yat-sen University,Guangzhou 510275,China [2]Institute of Advanced Wear&Corrosion Resistant and Functional Materials,Jinan University,Guangzhou 510632,China [3]Fine Chemical Industry Research Institute,School of Chemical Engineering and Technology,Sun Yat-sen University,Zhuhai 519082,China [4]School of Chemical Engineering,Guangdong University of Petrochemical Technology,Maoming 525000,China

出　　处：《Science China Chemistry》2020年第6期810-817,共8页中国科学（化学英文版）

基　　金：supported by the National Natural Science Foundation of China(21938001、21606260、21576302、21376278、21425627、21701199);the National Natural Science Foundation of ChinaSINOPEC Joint Fund(U1663220);the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(2017BT01C102);the Natural Science Foundation of Guang-dong Province(2015A030313104);the Fundamental Research Funds for the Central Universities of Sun Yat-sen University(15lgjc33、19lgpy129)。

摘　　要：Recently,nitrogen-doped porous carbon supported single atom catalysts(SACs)have become one of the most promising alternatives to precious metal catalysts in oxygen reduction reaction(ORR)due to their outstanding performance,especially those derived from porphyrin-based materials.However,most of them involve other metal residuals,which would cause the tedious pre-and/or post-treatment,even mislead the mechanistic investigations and active-site identification.Herein,we report a precursor-dilution strategy to synthesize Fe SACs through the Schiff-based reaction via co-polycondensation of amino-metalloporphyrin,followed by pyrolysis at high temperature.Systematic characterization results provide the compelling evidence of the dominant presence of atomically dispersed Fe-Nxspecies.Our catalyst shows superior ORR performance with positive half-wave potential(E1/2=0.85 V vs.RHE)in alkaline condition and moderate activity(E1/2=0.68 V vs.RHE)under the acidic condition,excellent methanol tolerance and good long-term stability.All the results indicate Fe SACs would be a promising candidate for replacing the precious Pt in metal-air batteries and fuel cells.

关 键 词：single atom catalysts PORPHYRIN precursor-dilution oxygen reduction reaction active site 

分 类 号：O643.36[理学—物理化学]