Separator modification with a high-entropy hydroxyphosphate, Co_0.29Ni_0.15Fe_0.33Cu_0.16Ca_3.9(PO₄)₃(OH), for high-performance Li-S batteries.

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2025-02-01 Epub Date: 2024-10-12 DOI:10.1016/j.jcis.2024.10.058

Xinyuan Wang, Yuxin Fan, Lei Xie, Huibing He, Guifang Wang, Jinliang Zhu

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Abstract

The shuttle effect of lithium polysulfides (LiPSs) significantly hinders the practical application of lithium-sulfur batteries (LSBs). Herein, a high-entropy hydroxyphosphate (Co_0.29Ni_0.15Fe_0.33Cu_0.16Ca_3.9(PO₄)₃(OH), denoted as HE-CHP), was synthesized by metal cation exchange with calcium hydroxyphosphate (CHP) and then coated on polypropylene (PP) separators to suppress the shuttling of LiPSs. Density functional theory calculations indicated that the various introduced metal cations could effectively modulate the binding strength of soluble polysulfides and enhance the reaction kinetics of LiPSs conversion. As a result, LSBs using the HE-CHP@PP separator exhibited an excellent discharge capacity (1297 mAh g^-1 under 0.2 C) and a slow capacity decay during long-term cycling (0.046 % per cycle at 2 C). At a sulfur loading of up to 6.5 mg cm^-2, the LSB with HE-CHP@PP separator displayed a discharge capacity of 5.8 mAh cm^-2. Notably, the CNT@S||Li Li-S pouch cell with HE-CHP modified separator delivered an initial energy density of 432 Wh kg^-1.

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使用高熵羟基磷酸盐 Co0.29Ni0.15Fe0.33Cu0.16Ca3.9(PO4)3(OH)对隔膜进行改性，用于高性能锂-S 电池。

多硫化锂（LiPSs）的穿梭效应严重阻碍了锂硫电池（LSBs）的实际应用。本文通过与羟基磷酸钙（CHP）进行金属阳离子交换合成了一种高熵羟基磷酸酯（Co0.29Ni0.15Fe0.33Cu0.16Ca3.9(PO4)3(OH)，简称 HE-CHP），然后涂覆在聚丙烯（PP）隔膜上以抑制多硫化锂的穿梭效应。密度泛函理论计算表明，引入的各种金属阳离子可有效调节可溶性多硫化物的结合强度，并增强锂离子多硫化物转化的反应动力学。因此，使用 HE-CHP@PP 分离剂的 LSB 具有出色的放电容量（0.2 C 下为 1297 mAh g-1），并且在长期循环过程中容量衰减缓慢（2 C 下每循环 0.046%）。当硫含量高达 6.5 mg cm-2 时，带有 HE-CHP@PP 隔离层的 LSB 显示出 5.8 mAh cm-2 的放电容量。值得注意的是，带有 HE-CHP 改良隔膜的 CNT@S||Li 锂-S 袋电池的初始能量密度为 432 Wh kg-1。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.