Polyphosphates-Based Cathode-Electrolyte Interphase for 4.65 V LiCoO2

Hengyu Ren

doi:10.1002/adma.73065

2026-04-16

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Feng Pan (Feng Pan) *

DOI：10.1002/adma.73065

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摘要

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锂钴氧（LCO）的稳定界面化学是其高压运行的基础。然而，源自钴/氧催化位点的界面副反应会导致碳酸亚乙酯（EC）氧化、六氟磷酸锂（LiPF6）水解以及LCO表面降解。在此，我们提出，电解质中功能性磷酸盐衍生物（FPD）的形成，这些衍生物由三（三甲基硅基）磷酸酯（TMSP）与PF6−阴离子反应生成，可以实现多磷酸盐正极-电解质界面（CEI）的靶向调控。在循环过程中，FPD自发与表面钴/氧位点形成共价相互作用，触发原位聚合，构建在LCO上形成坚固且全覆盖的CEI。所得CEI富含多磷酸盐和LiF/Li2O，同时确保高热力学稳定性和快速的Li+传输动力学。因此，采用优化电解液（1.0 M LiPF6在基于氟代碳酸亚乙酯（FEC）的溶剂中添加2.0 wt.% TMSP）的LCO展现出优异的电池性能，在3.0–4.6 V（vs. Li/Li+）电压范围内3000次循环后容量保持率为81.0%，在3.0–4.65 V范围内2000次循环后为81.6%，并在LCO||石墨软包电池中500次循环后保持率为80.0%，显示出其可行性。这项工作为通过功能电解液工程构建高压LCO正极的均匀CEI提供了新见解。

Keyword:

CEI

covalent interaction

high-voltage LiCoO2

polyphosphates

targeted construction

期刊

Advanced Materials

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26.8

论文数:

3.4W

被引数:

46.0W

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fujian normal university

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677

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peking university

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11.9W

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the university of hong kong

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1.0K

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被引数: 0

university of science and technology of china

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1.0W

论文数: 3.9K

被引数: 3

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