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高能锂电池的竞争性界面反应

 2026/6/21 10:16:40 《最新论文》 作者:科学网 小柯机器人 我有话说(0人评论) 字体大小:+

近日,厦门大学廖洪钢团队揭示了高能锂电池的竞争性界面反应。2026年6月17日出版的《自然》杂志发表了这项成果。

固-液界面处的电荷转移在各种储能系统中起着关键作用,尤其是在反应物浓度动态变化的条件下。解析这些复杂的反应路径仍然是一项重大挑战,特别是在锂硫(Li–S)电池中,因为实现高能量密度需要高效转化高浓度的多硫化锂(LiPSs)。然而,在贫电解液条件下,人们对硫化锂(Li2S)沉积与溶解的调控机制仍知之甚少。

研究组利用原位液体池电子显微镜,直接观察到了电极–电解质界面处由浓度驱动的相分离。在这些高浓度界面层(HCILs)中,表面与溶液之间的竞争决定了电荷转移动力学,并最终控制Li2S在不同相界面的沉积行为。密度泛函理论(DFT)计算表明,LiPSs的聚集改变了分子几何构型、电子特性和轨道杂化,从而共同促进了通过高浓度LiPSs簇的电荷转移。

基于这些认识,研究组设计了优化电极以平衡界面反应路径,实现了快速充电(4 C,26.8 mA cm-2)并获得了超过400 Wh kg-1的高能量密度。这些发现提供了在实际工作条件下界面反应的机理理解,并为推进Li–S电池发展提供了设计策略。

附:英文原文

Title: Revealing competitive interfacial reactions in high-energy Li–S batteries

Author: Zhou, Shiyuan, Pei, Fei, Zheng, Qizheng, Li, Gen, Yi, Hongyuan, Chen, Linzhi, Tang, Shi, Kang, Qi, Yin, Zu-Wei, Liu, Sangui, Xiao, Liangping, Huang, Ling, Qiao, Yu, Huang, Yunhui, Sun, Shi-Gang, Liao, Hong-Gang

Issue&Volume: 2026-06-17

Abstract: Charge transfer at solid–liquid interfaces plays a critical role in various energy-storage systems1, particularly under dynamically varying reactant concentrations. Deciphering these intricate reaction pathways remains a substantial challenge, notably in lithium–sulfur (Li–S) batteries, in which achieving high energy density requires efficient conversion of highly concentrated lithium polysulfides (LiPSs)2,3. However, the mechanisms governing lithium sulfide (Li2S) deposition and dissolution under lean electrolyte conditions remain poorly understood. Here, using in situ liquid-cell electron microscopy, we directly visualize concentration-driven phase segregation at the electrode–electrolyte interface. Within these high-concentration interfacial layers (HCILs), competitive surface and solution dictate the charge-transfer dynamics and ultimately govern Li2S deposition at different phase boundaries. Density functional theory (DFT) calculations reveal that the aggregation of LiPSs alters molecular geometry, electronic properties and orbital hybridization, collectively facilitating charge transfer through highly concentrated LiPSs clusters. Guided by these insights, we design optimized electrodes that balance interfacial reaction pathways, enabling fast charging (4C, 26.8mAcm2) and achieving high energy densities exceeding 400Whkg1. These findings provide mechanistic understanding of interfacial reactions under practical working conditions and offer a design strategy to advance Li–S batteries.

DOI: 10.1038/s41586-025-09473-2

Source: https://www.nature.com/articles/s41586-025-09473-2

期刊信息

Nature:《自然》,创刊于1869年。隶属于施普林格·自然出版集团,最新IF:69.504

官方网址:http://www.nature.com/

投稿链接:http://www.nature.com/authors/submit_manuscript.html

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