Mechanistic Study of Functional Electrolyte Solvents for High-Voltage Lithium Batteries

Hossain, Md Farhan; Abrha, Ljalem Hadush; Razzaq, Amir Abdul; Ogilvie, Regan; Dirks, William Charles; Studer, Haiden; Poches, Christopher; Lama, Bhubnesh; Oli, Himal; Bandlamudi, Santosh R. P.; Li, Xuguang; Pupek, Krzysztof; Yang, Zhenzhen; Paudel, Tula R.; Xing, Weibing

doi:10.1021/acsami.5c16368

Mechanistic Study of Functional Electrolyte Solvents for High-Voltage Lithium Batteries

Journal Article · Thu Oct 02 00:00:00 EDT 2025 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.5c16368· OSTI ID:2998908

Hossain, Md Farhan ^[1]; Abrha, Ljalem Hadush ^[1]; Razzaq, Amir Abdul ^[1]; Ogilvie, Regan ^[1]; Dirks, William Charles ^[1]; Studer, Haiden ^[1]; Poches, Christopher ^[1]; Lama, Bhubnesh ^[1]; ^[1]; Bandlamudi, Santosh R. P. ^[1]; Li, Xuguang ^[2]; Pupek, Krzysztof ^[3]; ^[3]; ^[1]; ^[1]

South Dakota School of Mines and Technology, Rapid City, SD (United States)
Lynntech Inc., College Station, TX (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)

The pervasive use of Ni-rich cathode active materials, e.g., LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811), for high-energy-density Li-ion batteries (LIBs) has been hindered by rapid battery capacity decay when cycled with high charge cutoff voltages due to electrolyte decomposition in the conventional carbonate solvent-based electrolytes, oxidative parasitic side reactions at the electrolyte/cathode interface, and irreversible phase changes in the cathode active materials leading to dissolution of transition metals into the electrolytes. Various functional electrolyte solvents have been studied to tackle the above technical challenges, yet the roles of individual solvents in the performance of LIBs remain poorly understood. Here, in this study, we systematically investigate electrochemical performance mechanisms of fluorinated and organosilicon single solvents and cosolvents, for the first time, in high-voltage Li/NMC811 batteries, using electrochemical and analytical characterizations and density functional theory modeling. We observe that some unique combinations of the functional solvents can lead to exceptionally stable high-voltage cycle performance in the Ni-rich cathode-based LIBs. Our mechanistic study reveals that the synergistic effect of solvents plays a vital role in enabling electrochemical stability at both the Ni-rich cathode and the Li metal anode. Understanding the electrochemical performance mechanisms of functional solvents can greatly help in designing and formulating advanced electrolytes that enable the development of high-voltage, high-energy-density, long-cycle-life lithium batteries.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Aeronautics and Space Administration (NASA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2998908

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 41 Vol. 17; ISSN 1944-8244; ISSN 1944-8252

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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