首页|Electronic structure and spin state regulation of vanadium nitride via a sulfur doping strategy toward flexible zinc-air batteries

Electronic structure and spin state regulation of vanadium nitride via a sulfur doping strategy toward flexible zinc-air batteries

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Owing to the distinctive structural characteristics,vanadium nitride(VN)is highly regarded as a catalyst for oxygen reduction reaction(ORR)in zinc-air batteries(ZABs).However,VN exhibits limited intrinsic ORR activity due to the weak adsorption ability to O-containing species.Here,the S-doped VN anchored on N,S-doped multi-dimensional carbon(S-VN/Co/NS-MC)was constructed using the solvothermal and in-situ doping methods.Incorporating sulfur atoms into VN species alters the electron spin state of vana-dium in the S-VN/Co/NS-MC for regulating the adsorption energy of vanadium sites to oxygen molecules.The introduced sulfur atoms polarize the V 3dz2 electrons,shifting spin-down electrons closer to the Fermi level in the S-VN/Co/NS-MC.Consequently,the introduction of sulfur atoms into VN species enhances the adsorption energy of vanadium sites for oxygen molecules.The*OOH dissociation transi-tions from being unspontaneous on the VN surface to a spontaneous state on the S-doped VN surface.Then,the ORR barrier on the S-VN/Co/NS-MC surface is reduced.The S-VN/Co/NS-MC demonstrates a higher half-wave potential and limiting current density compared to the VN/Co/N-MC.The S-VN/Co/NS-MC-based liquid ZABs display a power density of 195.7 mW cm-2,a specific capacity of 815.7 mA h g-1,and a cycling stability exceeding 250 h.The S-VN/Co/NS-MC-based flexible ZABs are suc-cessfully employed to charge both a smart watch and a mobile phone.This approach holds promise for advancing the commercial utilization of VN-based catalysts in ZABs.

S-doped VNElectronic structuresSpin state regulationOxygen reduction reactionZinc-air batteries

Daijie Deng、Honghui Zhang、Jianchun Wu、Xing Tang、Min Ling、Sihua Dong、Li Xu、Henan Li、Huaming Li

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Institute for Energy Research,Institute of Quantum and Sustainable Technology,School of Chemistry and Chemical Engineering,School of Materials Science and Engineering,Jiangsu Province and Education Ministry Co-Sponsored Synergistic Innovation Center of Modern Agricultural Equipment,Jiangsu University,Zhenjiang 212013,Jiangsu,China

Key Laboratory of Radio Frequency and Micro-Nano Electronics of Jiangsu Province,Nanjing 210023,Jiangsu,China

Zhenjiang Kangyuan Electrical Appliance Co.,Ltd.,Zhenjiang 212013,Jiangsu,China

College of Chemical and Biological Engineering,Zhejiang University,Hangzhou 310027,Zhejiang,China

YTO Group Corporation Dongfanghong(Henan)Agricultural Service Technology Co.,Ltd.,Luoyang 471033,Henan,China

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National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaJiangsu Province and Education Ministry Co-Sponsored Synergistic Innovation Center of Modern Agricultural EquipmentPriority Academic Program Development of Jiangsu Higher Education InstitutionsPostgraduate Research & Practice Innovation Program of Jiangsu Province

221781482227819322075113XTCX2029KYCX22_3691

2024

10.1016/j.jechem.2023.10.024

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)：2024.89(2)
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