Solvent Anchoring Coupled with Robust Interphase Construction for Stable Polymeric Lithium Metal Batteries

LU Yibo; ZHOU Tao; ZHANG Hao; XUE Xinjie; DENG Tao; ZHAO Changying

doi:10.19799/j.cnki.2095-4239.2026.0274

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Solvent Anchoring Coupled with Robust Interphase Construction for Stable Polymeric Lithium Metal Batteries

更新时间：2026-05-06

- Solvent Anchoring Coupled with Robust Interphase Construction for Stable Polymeric Lithium Metal Batteries
- Energy Storage Science and Technology Pages: 1-16(2026)
- 作者机构：
  
  1.上海交通大学中英国际低碳学院，上海 201306
  2.上海交通大学工程热物理研究所，上海 200240
- 作者简介：
- 基金信息：
- DOI：10.19799/j.cnki.2095-4239.2026.0274
  CLC： TM912
- Received：01 April 2026，
  
  Revised：2026-04-16，
  
  Online First：21 April 2026，
- 稿件说明：
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陆一波, 周涛, 张浩, 等. 溶剂锚定与界面强化协同构筑稳定聚合物锂金属电池[J]. 储能科学与技术, XXXX, XX(XX): 1-16.

LU Yibo, ZHOU Tao, ZHANG Hao, et al. Solvent Anchoring Coupled with Robust Interphase Construction for Stable Polymeric Lithium Metal Batteries[J]. Energy Storage Science and Technology, XXXX, XX(XX): 1-16.
陆一波, 周涛, 张浩, 等. 溶剂锚定与界面强化协同构筑稳定聚合物锂金属电池[J]. 储能科学与技术, XXXX, XX(XX): 1-16. DOI： 10.19799/j.cnki.2095-4239.2026.0274.

LU Yibo, ZHOU Tao, ZHANG Hao, et al. Solvent Anchoring Coupled with Robust Interphase Construction for Stable Polymeric Lithium Metal Batteries[J]. Energy Storage Science and Technology, XXXX, XX(XX): 1-16. DOI： 10.19799/j.cnki.2095-4239.2026.0274.

摘要

聚偏氟乙烯（PVDF）基聚合物电解质在固态锂金属电池（SSLMB）领域具有巨大的潜力，但它们的实际应用受到制备过程中残留溶剂N，N-二甲基甲酰胺（DMF）的限制。残留的DMF虽然可确保快速的离子传输，但其与锂金属剧烈的副反应严重损害了负极稳定性。本工作提出添加剂-填料协同的溶剂锚定策略，将离子液体1-丁基-3-甲基咪唑硝酸盐（[BMIM

]

[NO

]

）、硼酸锌（Zn

，ZB）和多功能陶瓷填料Li

6.4

1.4

0.6

（LLZTO）引入PVDF基聚合物，制备了一种厚度为40 μm的固态复合电解质薄膜（PBZL）。通过密度泛函理论（DFT）计算和分子动力学（MD）模拟，ZB和LLZTO对残留的DMF分子展现出极强的吸附作用，抑制其向电极侧迁移并减轻界面副反应。[BMIM

]

[NO

]

的引入使NO

阴离子进入Li

的初级溶剂化壳，从而削弱Li

-DMF配位；并且在负极优先被还原，促进富含无机物的固态电解质界面（SEI）的形成。得益于形成了富含LiF、Li

N、Li-Zn合金的坚固SEI，组装的Li|PBZL|Li对称电池在0.3 mA/cm

电流密度下能稳定循环2000小时以上，其循环寿命远超未改性的PVDF锂对称电池（30小时）。此外，LiNi

0.8

0.1

|PBZL|Li电池在30℃、0.5 C下循环200圈后，放电比容量高达162.1 mAh/g，容量保持率为90.2%，并且在倍率性能测试中2 C下仍能提供138.7 mAh/g的放电比容量，展现出优越的循环稳定性及倍率性能。本工作强调了溶剂锚定与界面强化是稳定锂金属负极、构筑高性能聚合物固态电池的关键策略。

Abstract

Polyvinylidene fluoride (PVDF)-based polymer electrolytes hold significant potential for solid-state lithium metal batteries (SSLMBs)

yet their practical deployment is hindered by residual N

N-dimethylformamide (DMF) originating from the preparation process. Specifically

while residual DMF ensures rapid ionic transport

it triggers severe interfacial side reactions with lithium metal

substantially compromising anode stability. Herein

we propose an additive-filler synergistic strategy integrating ionic liquid (1-butyl-3-methylimidazolium nitrate

[BMIM

]

[NO

]

)

zinc borate (Zn

ZB) and multifunctional ceramic fillers Li

6.4

1.4

0.6

(LLZTO) to anchor DMF

and fabricate a solid composite electrolyte membrane (denoted as PBZL) with a thickness of 40 μm. Density functional theory (DFT) calculations and molecular dynamics (MD) simulations reveal that ZB and LLZTO exhibit strong adsorption interactions with residual DMF molecules

suppressing their migration toward the electrode and mitigating interfacial side reactions. The introduction of [BMIM

]

[NO

]

allows NO

- anions to enter the primary solvation shell of Li

ther

eby weakening the Li

- DMF coordination. And it is preferentially reduced at the anode

promoting the formation of a solid electrolyte interface (SEI) rich in inorganic substances. Benefiting from the formation of a robust SEI rich in LiF/Li

N/Li-Zn alloy

the assembled Li|PBZL|Li symmetric cells stably cycle over 2000 h at 0.3 mA/cm

significantly outperforming the unmodified Li|PVDF|Li symmetric cells (30 h) under the same conditions. Furthermore

LiNi

0.8

0.1

||Li cells deliver a high discharge capacity of 162.1 mAh/g and maintain 90.2% capacity retention after 200 cycles at 0.5 C and 30 ℃

and exhibit a discharge capacity of 138.7 mAh/g at 2 C in the rate capability test

demonstrating excellent cycling stability and rate performance. This work highlights solvent anchoring coupled with interface reinforcement as critical approaches for stabilizing lithium metal anode and enabling high-performance polymeric SSLMBs.

关键词

Keywords

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