Stabilizing Graphite Anode in Electrolytes with Nanoscale Anion Networking for High-Rate Lithium Storage

Yu, Yikang; Xu, Jiayi; Duanmu, Kaining; Shutthanandan, Vaithiyalingam; Wi, Sungun; Yang, Zhenzhen; Liu, Yuzi; Lyu, Xingyi; Qian, Kun; Agarwal, Mangilal; Zhang, Zhengcheng; Zhang, Yugang; Li, Tao; Liu, Cong; Murugesan, Vijayakumar; Xie, Jian

doi:10.1021/acsenergylett.4c02011

Stabilizing Graphite Anode in Electrolytes with Nanoscale Anion Networking for High-Rate Lithium Storage

Journal Article · Fri Sep 20 00:00:00 EDT 2024 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.4c02011· OSTI ID:2475474

^[1]; ^[2]; ^[3]; ^[3]; Wi, Sungun ^[3]; ^[2]; ^[4]; ^[5]; Qian, Kun ^[5]; ^[6]; ^[2]; Zhang, Yugang ^[7]; ^[8]; ^[2]; ^[3]; ^[1]

Purdue Univ., West Lafayette, IN (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
Northern Illinois Univ., DeKalb, IL (United States)
Indiana University, Indianapolis IN (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Northern Illinois Univ., DeKalb, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Graphite is the preferred anode material in commercial lithium-ion batteries (LIBs), but its limited compatibility with various organic molecules restricts the electrolyte solvent options. The primary challenge is solvent co-intercalation with Li ions, leading to graphite layer exfoliation. As a result, electrolyte selection often relies on ethylene carbonate (EC)-based solvents. Here, in this study, we introduce electrolytes featuring a nanoscale anion network ordering that hinders the liquid-phase exfoliation of graphite. This network, formed from concentrated long-chain lithium salts, traps free dioxolane (DOL) molecules, reducing the interactions between graphite particles and solvents during Li intercalation. Our findings reveal a mechanism that stabilizes graphite in otherwise unstable solvents with concentrated salts like LiTFSI, providing key insights for improving LIB performance by addressing electrolyte limitations on graphite anodes.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: SC0012704; AC02-06CH11357

OSTI ID:: 2475474

Alternate ID(s):: OSTI ID: 2511209

Report Number(s):: BNL--226276-2024-JAAM

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 10 Vol. 9; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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