Synchronized Breathing in Anion-Derived Interphases

Tan, Sha; Xia, Kangxuan; Wang, Nan; Yen, Dean; Yu, Zhiao; Rahman, Muhammad Mominur; Chen, Xiaobo; Chen, Yuelang; Yang, Xiao-Qing; Xiao, Jie; Liu, Jun; Cui, Yi; Bao, Zhenan; Hu, Enyuan

doi:10.1021/acsenergylett.5c01756

Synchronized Breathing in Anion-Derived Interphases

Journal Article · Sat Jul 12 00:00:00 EDT 2025 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.5c01756· OSTI ID:2574074

^[1]; Xia, Kangxuan ^[1]; ^[1]; Yen, Dean ^[1]; ^[2]; Rahman, Muhammad Mominur ^[1]; Chen, Xiaobo ^[3]; ^[2]; ^[1]; ^[4]; ^[4]; ^[5]; ^[2]; ^[1]

Brookhaven National Laboratory (BNL), Upton, NY (United States)
Stanford Univ., CA (United States)
Univ. of Pittsburgh, PA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)

Anion-derived interphases are crucial for extending the cycle life of lithium metal batteries. While their benefits are often attributed to crystalline inorganic species like LiF and Li₂O, the role of amorphous inorganic species and the interplay between the anode-electrolyte interphase (SEI) and the cathode-electrolyte interphase (CEI) remain largely unexplored. Here, in this study, we examine two model electrolyte systems─one with solvent-derived interphases and the other with anion-derived interphases─using advanced X-ray scattering and spectroscopy techniques. Our findings reveal that anion-derived interphases contain substantial amounts of amorphous inorganic species, leading to a unique synchronization of "breathing" between SEI and CEI. During charging, the SEI grows while the CEI shrinks; during discharging, these roles reverse. This distinctive interfacial behavior originates from the competition of deposition and dissolution of amorphous inorganics during cycling. The study highlights the unique role of amorphous inorganics in anion-derived interphases, providing new insights into improving battery performance and durability.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2574074

Report Number(s):: BNL--228478-2025-JAAM

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 8 Vol. 10; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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