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在异质界面构建自发内建电场,实现多硫化物的持续高效吸附-定向迁移-转化。

Construction of spontaneous built-in electric field on heterointerface furnishing continuous efficient adsorption-directional migration-conversion of polysulfides.

作者信息

Xu Junwei, Wang Shuai, Zhou Haihui, Sun Jiale, Liu Xuying, Feng Wei, Guo Tingting, Gao Yuancan, Huang Zhongyuan

机构信息

State Key Laboratory for Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China.

State Key Laboratory for Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China.

出版信息

J Colloid Interface Sci. 2025 Mar 15;682:491-501. doi: 10.1016/j.jcis.2024.11.156. Epub 2024 Nov 29.

DOI:10.1016/j.jcis.2024.11.156
PMID:39637646
Abstract

Integrating sulfur with efficient electrocatalysts remains a pressing need in lithium-sulfur (Li-S) batteries for modulating the sluggish conversion kinetics and restricting the shuttle behavior of lithium polysulfides (LiPSs). Herein, a compact p-type FeO and n-type MoS heterostructure embedded on nitrogen-doped porous carbon (FeO-MoS-NPC-0.5) is meticulously constructed as dual-functional hosts that can facilitate continuous catalytic conversion of LiPSs. The p-type FeO exhibits a high affinity for polysulfides, while n-type MoS enables effective catalysis of LiPSs. The successful migration of LiPSs from FeO to MoS is bridged due to a spontaneous built-in electric field (BIEF) at the p-n heterojunction interface. The synergistic effect prevents the passivation of adsorption sites on FeO and enhances the efficient catalytic conversion capabilities of MoS. Consequently, the battery with FeO-MoS-NPC-0.5/S exhibits a prominent initial capacity of 1120.6 mAh g at 2 C, maintains outstanding cyclability with a capacity attenuation rate of 0.045 % per cycle at 0.5 C, and high sulfur utilization at large sulfur loadings. This work offers insights into optimizing the performance-enhanced Li-S battery electrodes by the formation of a dynamic "trapping-directional migration-conversion" reaction.

摘要

在锂硫(Li-S)电池中,将硫与高效电催化剂相结合仍然是一项迫切需求,以调节缓慢的转化动力学并限制多硫化锂(LiPSs)的穿梭行为。在此,一种嵌入氮掺杂多孔碳的致密p型FeO和n型MoS异质结构(FeO-MoS-NPC-0.5)被精心构建为双功能主体,可促进LiPSs的连续催化转化。p型FeO对多硫化物表现出高亲和力,而n型MoS能够有效催化LiPSs。由于p-n异质结界面处的自发内建电场(BIEF),LiPSs从FeO到MoS的成功迁移得以实现。这种协同效应防止了FeO上吸附位点的钝化,并增强了MoS的高效催化转化能力。因此,具有FeO-MoS-NPC-0.5/S的电池在2 C时表现出1120.6 mAh g的突出初始容量,在0.5 C时以每循环0.045%的容量衰减率保持出色的循环稳定性,并在高硫负载下具有高硫利用率。这项工作为通过形成动态的“捕获-定向迁移-转化”反应来优化性能增强的Li-S电池电极提供了见解。

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