Atomically dispersed Fe sites on hierarchically porous carbon nanoplates for oxygen reduction reaction

查看全文 作　　者：Ruixue [1,2,3]Zheng;Qinglei [1,3]Meng;Hao [4]Zhang;Teng [2,5]Li;Di [1,3]Yang;Li [1]Zhang;Xiaolong [1,2,3]Jia;Changpeng [1,2,3]Liu;Jianbing [1,2,3]Zhu;Xiaozheng [2,5]Duan;Meiling [1,2,3]Xiao;Wei [1,2,3]Xing 机构地区：[1]State Key Laboratory of Electroanalytical Chemistry,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,Jilin,China;[2]School of Applied Chemistry and Engineering,University of Science and Technology of China,Hefei 230026,Anhui,China;[3]Laboratory of Advanced Power Sources,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,Jilin,China;[4]Institute of Functional Nano&Soft Materials(FUNSOM),Jiangsu Key Laboratory for Carbon-Based Functional Materials&Devices,Jiangsu Key Laboratory of Advanced Negative Carbon Technologies,Soochow University,Suzhou 215123,Jiangsu,China;[5]State Key Laboratory of Polymer Physics and Chemistry,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,Jilin,China 出　　处：《Journal of Energy Chemistry》索引2024年第90卷第3期,共10页 基　　金：financially supported by the National Key R&D Program of China(2022YFB4004100);the National Natural Science Foundation of China(22272161);the Jilin Province Science and Technology Development Program(20230101367JC);financially supported by the National Natural Science Foundation of China(22073094);the Science and Technology Development Program of Jilin Province(20210402059GH);the Science and Technology Plan Projects of Yunnan Province(202101BC070001–007);the Major Science and Technology Projects for Independent Innovation of China FAW Group Co.,Ltd(20220301018GX);the essential support of the Network and Computing Center,CIAC,CAS;the Computing Center of Jilin Province。 摘　　要：Developing cost-effective,robust and stable non-precious metal catalysts for oxygen reduction reaction(ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air batteries.Although Fe-N-C single atom catalysts(SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N_(4) sites,they suffer from serious mass transport limitations as microporous templates/substrates,i.e.,zeolitic imidazolate frameworks(ZIFs),are usually employed to host the active sites.Motivated by this challenge,we herein develop a hydrogen-bonded organic framework(HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N_(4) sites.Such a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid(NH_(2)-BDC) and p-phenylenediamine(PDA) as both soft templates and C,N precursors.Benefitting from the structural merits inherited from HOF templates,the optimized catalyst(denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V(vs.reversible hydrogen electrode(RHE)) and a small overpotential of 356 mV at 10 mA cm^(-2) for the oxygen evolution reaction(OER).More excitingly,its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge-discharge gap of 0.72 V after 160 h.Molecular dynamics(MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O_(2),thus enhancing the ORR performance.In situ Raman results further indicate that the conversion of O_(2) to~*O_(2)-the rate-determining step(RDS) for Fe-N-C SAC-950.This work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties. 关 键 词：Fe single atom catalysts Oxygen reduction reaction Mesoporous structure Active sites Zinc-air battery