Electronic structure and spin state regulation of vanadium nitride via a sulfur doping strategy toward flexible zinc-air batteries
JOURNAL OF ENERGY CHEMISTRY(2024)
摘要
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. (c) 2023 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
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关键词
S-doped VN,Electronic structures,Spin state regulation,Oxygen reduction reaction,Zinc-air batteries
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