An unwanted guest in the electrochemical oxidation of high-voltage Li-ion battery electrolytes: the life of highly reactive protons

Ilic, Stefan; Martins, Milena; Liu, Haoyu; Martins, Pedro Farinazzo Bergamo Dias; Haering, Dominik; Yang, Jingtian; Hatsukade, Toru; Genorio, Bostjan; Weitzner, Stephen E.; Wan, Liwen F.; Zhang, Zhengcheng; Connell, Justin G.; Key, Baris; Cabana, Jordi; Strmcnik, Dusan

doi:10.1039/d5ee02403j

Title: An unwanted guest in the electrochemical oxidation of high-voltage Li-ion battery electrolytes: the life of highly reactive protons

Journal Article · Thu Jul 24 00:00:00 UTC 2025 · Energy & Environmental Science

DOI: https://doi.org/10.1039/d5ee02403j · OSTI ID:2587843

^[1]; Martins, Milena ^[2]; Liu, Haoyu ^[1]; Martins, Pedro Farinazzo Bergamo Dias ^[3];

^[1]; Yang, Jingtian ^[1]; Hatsukade, Toru ^[1];

^[4];

^[5];

^[1];

^[1]; Key, Baris ^[1];

^[1];

^[3]

Argonne National Laboratory (ANL), Argonne, IL (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States); National Institute of Chemistry (NIC), Ljubljana (Slovenia); University of Maribor (Slovenia)
Argonne National Laboratory (ANL), Argonne, IL (United States); National Institute of Chemistry (NIC), Ljubljana (Slovenia)
University of Ljubljana (Slovenia)
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States). Laboratory for Energy Applications for the Future (LEAF)

Lithium-ion batteries (LIBs) are central to the urgent societal need to decarbonize both transportation and energy storage on the grid. Unfortunately, despite their attractive energy/power density, as well as high coulombic and energy efficiencies, further improvement of this technology – especially their durability – is desperately needed. To support these efforts, our study focuses on fundamental understanding of the decomposition pathways for LIB electrolytes at the cathode–electrolyte interface (CEI), as the nature of these reactions directly controls the extent to which cell capacity and voltage decays in these systems. In this study, we employ electrochemical methods, coupled with product analysis using NMR spectroscopy and mass spectrometry, to determine the decomposition mechanisms in both model and technologically relevant electrolytes. Remarkably, we discovered the electrochemical formation of protons with high chemical activity, comparable to known superacids, at potentials relevant to practical Li-ion batteries. Their reactivity toward every individual component of the CEI provides a unified thermochemical origin for a myriad of side reactions that are commonly associated with the electrochemical reaction. In particular, electrochemically generated protons react with intact EC molecules to form CO₂ and other short and long chain ethers. They also undergo an acid–base reaction with LiPF₆, to form the weaker acid HF, and with the cathode active material, leaching transition metals into the electrolyte. Collectively, the results of this study all point to the urgent need to either mitigate this proton formation or introduce benign harvesting additives via new electrolyte design strategies.

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Research Organization:: Argonne National Laboratory (ANL); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: Slovenian Research and Innovation Agency (ARIS); The Slovenian Research and Innovation Agency; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC); Vehicle Technologies Office

Grant/Contract Number:: AC02-06CH11357; AC52-07NA27344

OSTI ID:: 2587843

Report Number(s):: LLNL--JRNL-864706

Journal Information:: Energy & Environmental Science, Journal Name: Energy & Environmental Science Journal Issue: 17 Vol. 18; ISSN 1754-5706; ISSN 1754-5692

Publisher:: Royal Society of Chemistry (RSC)Copyright Statement

Country of Publication:: United States

Language:: English

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