Speciation of Transition Metal Dissolution in Electrolyte from Common Cathode Materials

Rynearson, Leah; Antolini, Cali; Jayawardana, Chamithri; Yeddala, Munaiah; Hayes, Dugan; Lucht, Brett L.

doi:10.1002/ange.202317109

Title: Speciation of Transition Metal Dissolution in Electrolyte from Common Cathode Materials

Journal Article · 20 December 2023 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.202317109 · OSTI ID:2263329

Rynearson, Leah ^[1]; Antolini, Cali ^[1]; Jayawardana, Chamithri ^[1]; Yeddala, Munaiah ^[1]; Hayes, Dugan ^[1];

^[1]

Department of Chemistry University of Rhode Island Kingston RI-02881 USA

Abstract Significant capacity loss has been observed across extended cycling of lithium‐ion batteries cycled to high potential. One of the sources of capacity fade is transition metal dissolution from the cathode active material, ion migration through the electrolyte, and deposition on the solid‐electrolyte interphase on the anode. While much research has been conducted on the oxidation state of the transition metal in the cathode active material or deposited on the anode, there have been limited investigations of the oxidation state of the transition metal ions dissolved in the electrolyte. In this work, X‐ray absorption spectroscopy has been performed on electrolytes extracted from cells built with four different cathode active materials (LiMn ₂ O ₄ (LMO), LiNi _0.5 Mn _1.5 O ₄ (LNMO), LiNi _0.8 Mn _0.1 Co _0.1 O ₂ (NMC811), and (x Li ₂ MnO ₃ *(1‐x) LiNi _a Mn _b Co _c O ₂ , with a+b+ c =1) (LMRNMC)) that were cycled at either high or standard potentials to determine the oxidation state of Mn and Ni in solution. Inductively coupled plasma‐mass spectrometry has been performed on the anodes from these cells to determine the concentration of deposited transition metal ions. While transition metal ions were found dissolved in all electrolytes, the oxidation state(s) of Mn and Ni were determined to be dependent on the cathode material and independent of cycling potential.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; SC0021392

OSTI ID:: 2263329

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 5 Vol. 136; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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