TY  - JOUR
AU  - Wang, Wei
AU  - Yu, Zhipeng
AU  - Yue, Liguo
AU  - Çaha, Ihsan
AU  - Zhang, Weicai
AU  - Chen, Qingqing
AU  - Huang, Haoliang
AU  - Lin, Fei
AU  - Zhao, Yang
AU  - Zeng, Jinfeng
AU  - Lu, Jingcheng
AU  - Deepak, Francis Leonard
AU  - Liu, Lifeng
TI  - Regulating Electronic Structure and Coordination Environment of Transition Metal Selenides through the High-Entropy Strategy for Expedited Lithium–Sulfur Chemistry
JO  - ACS nano
VL  - 19
IS  - 30
SN  - 1936-0851
CY  - Washington, DC
PB  - Soc.
M1  - PUBDB-2025-03725
SP  - 27440 - 27454
PY  - 2025
AB  - 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
LB  - PUB:(DE-HGF)16
DO  - DOI:10.1021/acsnano.5c05720
UR  - https://bib-pubdb1.desy.de/record/636994
ER  -