Hansen Wang, Xiaolin Yan, Rupeng Zhang, Juanjuan Sun, Fuxiang Feng, Haoran Li, Jinding Liang, Yuchun Wang, Guangzhou Ye, Xiaonan Luo, Shengyuan Huang, Pan Wan, Samantha T. Hung, Fangjun Ye, Fangyun Chen, Erxiao Wu, Jinfei Zhou, Ulderico Ulissi, Xiaoming Ge, Chengyong Liu, Bo Xu, Na Liu, Chuying Ouyang
{"title":"Application-driven design of non-aqueous electrolyte solutions through quantification of interfacial reactions in lithium metal batteries","authors":"Hansen Wang, Xiaolin Yan, Rupeng Zhang, Juanjuan Sun, Fuxiang Feng, Haoran Li, Jinding Liang, Yuchun Wang, Guangzhou Ye, Xiaonan Luo, Shengyuan Huang, Pan Wan, Samantha T. Hung, Fangjun Ye, Fangyun Chen, Erxiao Wu, Jinfei Zhou, Ulderico Ulissi, Xiaoming Ge, Chengyong Liu, Bo Xu, Na Liu, Chuying Ouyang","doi":"10.1038/s41565-025-01935-y","DOIUrl":null,"url":null,"abstract":"<p>Unwanted side reactions occurring at electrode|electrolyte interfaces significantly impact the cycling life of lithium metal batteries. However, a comprehensive view that rationalizes these interfacial reactions and assesses them both qualitatively and quantitatively is not yet established. Here, by combining multiple analytical techniques, we systematically investigate the interfacial reactions in lithium metal batteries containing ether-based non-aqueous electrolyte solutions. We quantitatively monitor various nanoscale-driven processes such as the reduction and oxidation pathways of lithium salt and organic solvents, the formation of various solid-electrolyte interphase species, the gas generation within the cell and the cross-talk processes between the electrodes. We demonstrate that the consumption of lithium ions owing to the continuous decomposition of the lithium bis(fluorosulfonyl)imide salt, which dominates the interfacial reactions, results in ion depletion during the cell discharge and battery failure. On the basis of these findings, we propose an electrolyte formulation in which lithium bis(fluorosulfonyl)imide content is maximized without compromising dynamic viscosity and bulk ionic conductivity, aiming for long-cycling battery performance. Following this strategy, we assemble and test Li (20 μm thickness)||LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.</sub><sub>1</sub>O<sub>2</sub> (17.1 mg cm<sup>−</sup><sup>2</sup> of active material) single-layer stack pouch cells in lean electrolyte conditions (that is, 2.1 g Ah<sup>−1</sup>), which can effectively sustain 483 charge (0.2 C or 28 mA)/discharge (1 C or 140 mA) cycles at 25 °C demonstrating a discharge capacity retention of about 77%.</p>","PeriodicalId":18915,"journal":{"name":"Nature nanotechnology","volume":"33 1","pages":""},"PeriodicalIF":38.1000,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature nanotechnology","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1038/s41565-025-01935-y","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Unwanted side reactions occurring at electrode|electrolyte interfaces significantly impact the cycling life of lithium metal batteries. However, a comprehensive view that rationalizes these interfacial reactions and assesses them both qualitatively and quantitatively is not yet established. Here, by combining multiple analytical techniques, we systematically investigate the interfacial reactions in lithium metal batteries containing ether-based non-aqueous electrolyte solutions. We quantitatively monitor various nanoscale-driven processes such as the reduction and oxidation pathways of lithium salt and organic solvents, the formation of various solid-electrolyte interphase species, the gas generation within the cell and the cross-talk processes between the electrodes. We demonstrate that the consumption of lithium ions owing to the continuous decomposition of the lithium bis(fluorosulfonyl)imide salt, which dominates the interfacial reactions, results in ion depletion during the cell discharge and battery failure. On the basis of these findings, we propose an electrolyte formulation in which lithium bis(fluorosulfonyl)imide content is maximized without compromising dynamic viscosity and bulk ionic conductivity, aiming for long-cycling battery performance. Following this strategy, we assemble and test Li (20 μm thickness)||LiNi0.8Mn0.1Co0.1O2 (17.1 mg cm−2 of active material) single-layer stack pouch cells in lean electrolyte conditions (that is, 2.1 g Ah−1), which can effectively sustain 483 charge (0.2 C or 28 mA)/discharge (1 C or 140 mA) cycles at 25 °C demonstrating a discharge capacity retention of about 77%.
期刊介绍:
Nature Nanotechnology is a prestigious journal that publishes high-quality papers in various areas of nanoscience and nanotechnology. The journal focuses on the design, characterization, and production of structures, devices, and systems that manipulate and control materials at atomic, molecular, and macromolecular scales. It encompasses both bottom-up and top-down approaches, as well as their combinations.
Furthermore, Nature Nanotechnology fosters the exchange of ideas among researchers from diverse disciplines such as chemistry, physics, material science, biomedical research, engineering, and more. It promotes collaboration at the forefront of this multidisciplinary field. The journal covers a wide range of topics, from fundamental research in physics, chemistry, and biology, including computational work and simulations, to the development of innovative devices and technologies for various industrial sectors such as information technology, medicine, manufacturing, high-performance materials, energy, and environmental technologies. It includes coverage of organic, inorganic, and hybrid materials.