Anchoring and Competition: Weakly Solvated Structure of Glymes Enhances Stability in Lithium Metal Batteries Operating under Extreme Conditions

Lithium metal batteries (LMBs) face challenges from unstable and fragile solid electrolyte interphases (SEIs). In this work, we successfully develop a novel electrolyte by effectively modulating the competitive solvation process in LMBs. In this formulation, the C─O─C motifs of glymes are competitively substituted by other anions and solvents to achieve single oxygen site coordination, thereby facilitating a weak solvation effect. At an apparent concentration of 1.25 M, a solvated sheath enriched with anions and single oxygen-bound complexes is formed, which significantly enhances lithium metal compatibility and promotes rapid desolvation kinetics. The designed electrolyte using weakly solvated structures exhibits remarkable stability at both 25° and 80 °C, enabling the lithium iron phosphate (LFP)||Li cell to achieve over 2000 cycles (capacity retention: 90%) and 500 cycles (capacity retention: 96%), respectively. Interestingly, the low N/P ratio LFP||Li (N/P = 1.8) full battery maintains a stable capacity over 50 cycles, and the commercial 1.1 Ah LFP||Li pouch cell shows a great stability (capacity retention: 91.0%, CE: 99.82%) over 20 cycles. The distinctive solvation regulation strategy has paved a novel research avenue for the realization of high-performance LMBs.

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Publication Details

Journal
Angewandte Chemie International Edition
Published
2025-08-14
DOI
https://doi.org/10.1002/anie.202511336
Citations
6
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
4.38

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article

Anchoring and Competition: Weakly Solvated Structure of Glymes Enhances Stability in Lithium Metal Batteries Operating under Extreme Conditions

Hongwei Yu, Weijie Guo, Xiaotang Shi, Zerui Li et al.
6 citations
Angewandte Chemie International Edition
Advancements in Battery Materials
4.38
article

Anchoring and Competition: Weakly Solvated Structure of Glymes Enhances Stability in Lithium Metal Batteries Operating under Extreme Conditions

Hongwei Yu, Weijie Guo, Xiaotang Shi, Zerui Li, Yongyao Xia, Ruoxuan Qi, Zhuijun Xu, Yuxin Liang, Jianwei Xiong, Yiyao Xiao, Guangjiu Pan, Xiaohong Li, Tonghui Xu, Ming Yang, Hongbin Zhao, Qingxiang Zeng, Tianle Zheng, Weiping Xie, Mengqi Wu, Yonggao Xia
article en
6 citations

Abstract

Lithium metal batteries (LMBs) face challenges from unstable and fragile solid electrolyte interphases (SEIs). In this work, we successfully develop a novel electrolyte by effectively modulating the competitive solvation process in LMBs. In this formulation, the C─O─C motifs of glymes are competitively substituted by other anions and solvents to achieve single oxygen site coordination, thereby facilitating a weak solvation effect. At an apparent concentration of 1.25 M, a solvated sheath enriched with anions and single oxygen-bound complexes is formed, which significantly enhances lithium metal compatibility and promotes rapid desolvation kinetics. The designed electrolyte using weakly solvated structures exhibits remarkable stability at both 25° and 80 °C, enabling the lithium iron phosphate (LFP)||Li cell to achieve over 2000 cycles (capacity retention: 90%) and 500 cycles (capacity retention: 96%), respectively. Interestingly, the low N/P ratio LFP||Li (N/P = 1.8) full battery maintains a stable capacity over 50 cycles, and the commercial 1.1 Ah LFP||Li pouch cell shows a great stability (capacity retention: 91.0%, CE: 99.82%) over 20 cycles. The distinctive solvation regulation strategy has paved a novel research avenue for the realization of high-performance LMBs.

Angewandte Chemie International EditionVol. 64(40)
Ningbo University (CN), Shanghai University (CN), Shanghai University of Engineering Science (CN), Ningbo University of Technology (CN), Hohai University (CN), Fudan University (CN), Soochow University (CN), University of Chinese Academy of Sciences (CN), Ningbo Institute of Industrial Technology (CN), Technical University of Munich (DE), Nanjing University of Aeronautics and Astronautics (CN)
Deutsche Forschungsgemeinschaft, National Natural Science Foundation of China, China Scholarship Council, Natural Science Foundation of Zhejiang Province
Openalex Percentile: Top 5%
Advancements in Battery Materials
4.38
DOIOpen Access PDFOpenAlex
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