Improving the electrocatalytic performances of Pt-based catalysts for oxygen reduction reaction via strong interactions with single-CoN_(4)-rich carbon support  

作　　者：Jin Long Xingqun Zheng Bin Wang Chenzhong Wu Qingmei Wang Lishan Peng 

机构地区：[1]Guizhou University Key Laboratory of Green Chemical and Clean Energy Technology,Guizhou University Engineering Research Center of Efficient Utilization for Industrial Waste,Institute of Dual-carbon and New Energy Technology Innovation and Development of Guizhou Province,School of Chemistry and Chemical Engineering,Guizhou University,Guiyang 550025,China [2]College of Safety Engineering,Chongqing University of Science&Technology,Chongqing 401331,China [3]Key Laboratory of Rare Earths,Chinese Academy of Sciences,Ganjiang Innovation Academy,Ganzhou 341119,China

出　　处：《Chinese Chemical Letters》2024年第5期265-271,共7页中国化学快报（英文版）

基　　金：financially supported by the Natural Science Foundation of China(Nos.22169005,22209186,22068009 and 22262006);the Science and Technology Support Project of Guizhou Provincial Science and Technology Department(Nos.ZK[2023]050 and[2023]403);the Open Project of Institute of Dualcarbon and New Energy Technology Innovation and Development of Guizhou Province(No.DCRE-2023-06);Youth Innovation Promotion Association,CAS(No.2023343);Self-deployed Projects of Ganjiang Innovation Academy,CAS(No.E355F006).

摘　　要：Developing platinum-group-metal(PGM)catalysts possessing strong metal-support interaction and controllable PGM size is urgent for the sluggish oxygen reduction reaction(ORR)in proton-exchange membrane fuel cells.Herein,we propose an in-situ self-assembled reduction strategy to successfully induce highly-dispersed sub-3nm platinum nanoparticles(Pt NPs)to attach on resin-derived atomic Co coordinated by N-doped carbon substrate(Pt/Co_(SA)-N-C)for ORR.To be specific,the interfacial electron interaction effect,along with a highly robust Co_(SA)-N-C support endow the as-fabricated Pt/Co_(SA)-N-C catalyst with significantly enhanced catalytic properties,i.e.,a mass activity(MA)of 0.719 A/mgPt at 0.9 ViR-free and a reduction of 24.2%in MA after a 20,000-cycles test.Density functional theory(DFT)calculations demonstrate that the enhanced electron interaction between Pt and Co_(SA)-N-C support decreases the dband center of Pt,which is in favor of lowering the desorption energy of ^(*)OH on Pt/Co_(SA)-N-C surface and accelerating the formation of H_(2)O,thus enhance the instinct activity of ORR.Furthermore,the higher binding energy between Pt and Co_(SA)-N-C compared to Pt and C indicates that the migration of Pt has been suppressed,which theoretically explains the improved durability of Pt/Co_(SA)-N-C.Our work offers an enlightenment on constructing composite Pt-based catalysts with multiple active sites.

关 键 词：Fuel cells Oxygen reduction reaction PLATINUM Single-CoN_(4)-rich carbon support Metal-substrate interaction 

分 类 号：TQ426[化学工程] TM911.4[电气工程—电力电子与电力传动]