Design of ZnSe-CoSe heterostructure decorated in hollow N-doped carbon nanocage with generous adsorption and catalysis sites for the reversibly fast kinetics of polysulfide conversion

doi:10.1016/j.jechem.2023.07.007

Abstract

Abstract: Although lithium-sulfur batteries (LiSBs) are regarded as one of the most promising candidates for the next-generation energy storage system, the actual industrial application is hindered by the sluggish solid-liquid phase conversion kinetics, severe shuttle effect, and low sulfur loadings. Herein, a zeolitic imidazolate framework (ZIF) derived heterogeneous ZnSe-CoSe nanoparticles encapsulated in hollow N-doped carbon nanocage (ZnSe-CoSe-HNC) was designed by etching with tannic acid as a multifunctional electrocatalyst to boost the polysulfide conversion kinetics in LiSBs. The hollow structure in ZIF ensures large inner voids for sulfur and buffering volume expansions. Abundant exposed ZnSe-CoSe heterogeneous interfaces serve as bifunctional adsorption-catalytic centers to accelerate the conversion kinetics and alleviate the shuttle effect. Together with the highly conductive framework, the ZnSe-CoSe-HNC/S cathode exhibits a high initial reversible capacity of 1305.3 mA h g^-1 at 0.2 C, high-rate capability, and reliable cycling stability under high sulfur loading and lean electrolyte (maintaining at 745 mA h g^-1 after 200 cycles with a high sulfur loading of 6.4 mg cm^-2 and a low electrolyte/sulfur ratio of 6 μL mg^-1). Theoretical calculations have demonstrated the heterostructures of ZnSe-CoSe offer higher binding energy to lithium polysulfides than that of ZnSe or CoSe, facilitating the electron transfer to lithium polysulfides. This work provides a novel heterostructure with superior catalytic ability and hollow conductive architecture, paving the way for the practical application of functional sulfur electrodes.

Key words: Lithium-sulfur batteries, Heterostructure, Conversion Kinetics, Hollow structure, Bi-directional catalysis

Junan Feng, Chuan Shi, Hanghang Dong, Chaoyue Zhang, Wendong Liu, Yu Liu, Tianyi Wang, Xiaoxian Zhao, Shuangqiang Chen, Jianjun Song. Design of ZnSe-CoSe heterostructure decorated in hollow N-doped carbon nanocage with generous adsorption and catalysis sites for the reversibly fast kinetics of polysulfide conversion[J]. Journal of Energy Chemistry, 2023, 86(11): 135-145.

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URL: https://www.jenergychem.com/EN/10.1016/j.jechem.2023.07.007

https://www.jenergychem.com/EN/Y2023/V86/I11/135

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