%0 Journal Article
%A Wang, Wei
%A Yu, Zhipeng
%A Yue, Liguo
%A Çaha, Ihsan
%A Zhang, Weicai
%A Chen, Qingqing
%A Huang, Haoliang
%A Lin, Fei
%A Zhao, Yang
%A Zeng, Jinfeng
%A Lu, Jingcheng
%A Deepak, Francis Leonard
%A Liu, Lifeng
%T Regulating Electronic Structure and Coordination Environment of Transition Metal Selenides through the High-Entropy Strategy for Expedited Lithium–Sulfur Chemistry
%J ACS nano
%V 19
%N 30
%@ 1936-0851
%C Washington, DC
%I Soc.
%M PUBDB-2025-03725
%P 27440 - 27454
%D 2025
%X Transition metal diselenides (TMSe<sub>2</sub>) have proven as promising catalysts able to promote the conversion kinetics of lithium polysulfides (LiPSs) in lithium–sulfur batteries (LSBs). However, the limited number of catalytically active edge sites in TMSe<sub>2</sub> severely hinders the realization of their full potential for boosting LSB’s performance. Herein, we report the synthesis of high-entropy NiCoMnCrVSe<sub>2</sub> nanoflakes anchored on graphene supports (NiCoMnCrVSe<sub>2</sub>/G) through a microwave-assisted solvothermal method. We systematically investigate how the high-entropy strategy enables the regulation of the electronic structure and coordination of various metal species in TMSe<sub>2</sub> through comprehensive experimental studies and theoretical calculations. Our results show that as the number of transition metals in TMSe<sub>2</sub> increases, the d-band center of metal active sites upshifts toward the Fermi level and the difference among d-band centers of various metal species diminishes, which facilitates the adsorption of LiPSs and lowers the energy barriers to nucleation/decomposition of Li<sub>2</sub>S. Consequently, LSBs containing NiCoMnCrVSe<sub>2</sub>/G as sulfur hosts deliver a high specific discharge capacity of 1453 mAh g<sup>–1</sup> at 0.1 C and excellent stability at 1 C for 500 cycles with a low decay rate of merely 0.016
%F PUB:(DE-HGF)16
%9 Journal Article
%R 10.1021/acsnano.5c05720
%U https://bib-pubdb1.desy.de/record/636994