High-Entropy Local Microenvironment-Catalyzed Tandem Reaction Achieves Superfast Sodium Storage Anode
Xuanlong He, Zhehao Zhao, Xiaodan Yang, Xingyue Liu, Ming Yang, Liang He, Zhu Jianhui, Yanyi Wang, Hongwei Mi, Lipeng Zhang, Chuanxin He, Dingtao Ma, Peixin Zhang
Abstract
Sodium-ion batteries hold promising application potential in the field of low-speed electric vehicles. However, the sluggish kinetics and poor thermodynamic stability of conventional sodium-ion battery anode materials limit their applicability under fast-charging and long-cycle conditions. Herein, we propose a high-entropy multicomponent interface design paradigm to tailoring a unique (TiVCrNbTa) 0.2 Se 2 (HE 0.2 Se 2 ) anode. Leveraging the synergistic catalytic effect among high-entropy atoms to catalyze the tandem reaction and enable rapid phase transitions. Theoretical calculations reveal that local microenvironment of the high-entropy intrinsic structure reduces adsorption energy and diffusion barriers at metal-Se sites, enhances Na-ion mobility, and improves metal-Se bonding, thereby catalyzing tandem reaction and accelerating phase transition. Ex situ Raman spectroscopy, in situ XRD, and AC-TEM analyses further confirm the thermodynamic reversibility of the HE 0.2 Se 2 electrode. At a high current density of 10 A g –1, HE 0.2 Se 2 delivers a specific capacity of 396.7 mAh g –1 after 1000 cycles. And delivering specific capacities exceeding 310 and 200.8 mAh g –1 at 50 A g –1 and 100 A g –1 . Full-cell testing demonstrates excellent cycling stability, with the capacity remaining stable after 400 cycles. This study provides essential theoretical insights and an experimental foundation for designing ultrafast-charging anodes applicable to a variety of energy storage systems.