Ether‐Oxygen Groups Modified Carboxylic Ester Enabling High‐Voltage Lithium Metal Batteries
Lithium metal batteries (LMBs) operating at high cut-off voltages can achieve an energy density exceeding 500 Wh kg<sup>-1</sup>; however, they often suffer from severe capacity degradation due to electrolyte decomposition. Herein, propylene glycol monomethyl ether acetate (PMA) is introduced as a novel solvent for LMB electrolytes. The unique ether-oxygen functionality in PMA exhibits high steric hindrance, leading to weak lithium-ion coordination, which promotes the formation of contact ion pairs (CIPs) in the electrolyte solvation structure, especially in the presence of dual salts. A Li||LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) battery employing the formulated PMA-based electrolyte demonstrates stable cycling at a high cut-off voltage of 4.5 V for over 100 cycles, retaining 90.1% of its initial capacity even at 60 °C. Furthermore, a molecular interfacial model is proposed to elucidate the impact of the designed electrolyte on electrode interfacial behavior and battery performance, providing valuable insights for the development of high-performance LMB electrolytes.
Authors
- Yinghua Chen (ORCID: https://orcid.org/0000-0001-6119-0061)
- Wandi Wahyudi (ORCID: https://orcid.org/0000-0002-6224-2414)
- Jun Ming (ORCID: https://orcid.org/0000-0001-9561-5718)
- Hui Zhu (ORCID: https://orcid.org/0000-0002-5935-4052)
- Qian Li (ORCID: https://orcid.org/0000-0002-3698-342X)
- Jiao Yin (ORCID: https://orcid.org/0000-0001-7196-9087)
- Akang Huang
- Jia Wang (ORCID: https://orcid.org/0009-0006-9377-8779)
- Shuang Li (ORCID: https://orcid.org/0000-0003-3647-9802)
- Pushpendra Kumar (ORCID: https://orcid.org/0000-0001-8920-2415)
- Zheng Ma
- Hongliang Xie
Institutions
- University of Science and Technology of China (CN)
- Jawaharlal Nehru University (IN)
- Chinese Academy of Sciences (CN)
- Changchun Institute of Applied Chemistry (CN)
- Xinjiang Technical Institute of Physics & Chemistry (CN)
- King Abdullah University of Science and Technology (SA)
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2025-05-23
- DOI
- https://doi.org/10.1002/anie.202504490
- Citations
- 11
- Primary Topic
- Advanced Battery Materials and Technologies
- Type
- article
- Field-Weighted Citation Impact
- 8.03
Funders
- National Natural Science Foundation of China
- People's Government of Jilin Province
- King Abdullah University of Science and Technology
- National Key Research and Development Program of China