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atomically dispersed fe sites on hierarchically porous carbon nanoplates for oxygen reduction reaction

Journal of Energy Chemistry 2024年第3期90卷 7-15,I0002页

作者： Ruixue Zheng Qinglei Meng Hao Zhang Teng Li Di Yang Li Zhang Xiaolong Jia Changpeng Liu Jianbing Zhu Xiaozheng Duan Meiling Xiao Wei Xing State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123JiangsuChina State Key Laboratory of Polymer Physics and Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina

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 *** 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 *** 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) *** 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 *** 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(*** 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 *** dynamics(MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O_(2),thus enhancing the ORR *** situ Raman results further indicate that the conversion of O_(2) to~*O_(2)-the rate-determining step(RDS) for fe-N-C *** 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

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Aqueous Zinc Batteries with Ultra‑Fast Redox Kinetics and High Iodine Utilization Enabled by Iron single atom catalysts

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Nano-Micro Letters 2023年第8期15卷 368-380页

作者： Xueya Yang Huiqing Fan Fulong Hu Shengmei Chen Kang Yan Longtao Ma State Key Laboratory of Solidification Processing School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072People’s Republic of China Frontiers Science Center for Flexible Electronics Institute of Flexible ElectronicsNorthwestern Polytechnical UniversityXi’an 710072People’s Republic of China Department of Materials Science and Engineering City University of Hong Kong83 Tat Chee AvenueKowloon 999077Hong KongPeople’s Republic of China

Rechargeable aqueous zinc iodine(ZnǀǀI_(2))batteries have been promising energy storage technologies due to low-cost position and constitutional safety of zinc anode,iodine cathode and aqueous ***,on one hand,the low-fraction utilization of electrochemically inert host causes severe shuttle of soluble polyiodides,deficient iodine utilization and sluggish reaction *** the other hand,the usage of high mass polar electrocatalysts occupies mass and volume of electrode materials and sacrifices device-level energy ***,we propose a“confinement-catalysis”host composed of fe single atom catalyst embedding inside ordered mesoporous carbon host,which can effectively confine and catalytically convert I_(2)/I^(−)couple and polyiodide ***,the cathode enables the high capacity of 188.2 mAh g^(−1)at 0.3 A g^(−1),excellent rate capability with a capacity of 139.6 mAh g^(−1)delivered at high current density of 15 A g^(−1)and ultra-long cyclic stability over 50,000 cycles with 80.5%initial capacity retained under high iodine loading of 76.72 wt%.Furthermore,the electrocatalytic host can also accelerate the I^(+)↔I_(2)*** greatly improved electrochemical performance originates from the modulation of physicochemical confinement and the decrease of energy barrier for reversible I−/I_(2)and I_(2)/I^(+)couples,and polyiodide intermediates conversions.

关键词： Aqueous zinc batteries Iodine reduction reaction fe single atom catalysts

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