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

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

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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-N4 sites,they suffer from serious mass transport limitations as microporous templates/substrates,i.e.,zeolitic imidazolate frame-works(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 hierarchi-cal micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N4 sites.Such a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid(NH2-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)dis-plays outstanding ORR activity with a high half-wave potential of 0.895 V(vs.reversible hydrogen elec-trode(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 O2,thus enhancing the ORR performance.In situ Raman results further indicate that the conversion of O2 to*O2-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.

Fe single atom catalystsOxygen reduction reactionMesoporous structureActive sitesZinc-air battery

Ruixue Zheng、Qinglei Meng、Hao Zhang、Teng Li、Di Yang、Li Zhang、Xiaolong Jia、Changpeng Liu、Jianbing Zhu、Xiaozheng Duan、Meiling Xiao、Wei Xing

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State Key Laboratory of Electroanalytical Chemistry,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,Jilin,China

School of Applied Chemistry and Engineering,University of Science and Technology of China,Hefei 230026,Anhui,China

Laboratory of Advanced Power Sources,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,Jilin,China

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

State Key Laboratory of Polymer Physics and Chemistry,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,Jilin,China

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国家重点研发计划国家自然科学基金吉林省科技发展计划Shanghai Synchrotron Radiation Facility国家自然科学基金吉林省科技发展计划Science and Technology Plan Projects of Yunnan ProvinceMajor Science and Technology Projects for Independent Innovation of China FAW Group Co.,LtdNetwork and Computing Center,CIAC,CASComputing Center of Jilin Province

2022YFB40041002227216120230101367JC2207309420210402059GH202101BC070001-00720220301018GX

2024

10.1016/j.jechem.2023.10.045

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.90(3)
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