Compositionally Complex Spinel Oxides as Conversion Anodes for Lithium-Ion Batteries

Four different compositionally complex multicomponent M<sub>3</sub>O<sub>4</sub> spinels containing 5-8 distinct metals were prepared by a rapid combustion synthesis method or solvothermal synthesis. High resolution synchrotron X-ray diffraction patterns show that the materials consist primarily of spinel phases with small amounts of rock salt impurities, and, in several samples, a minor amount of contracted spinel phase. Materials were investigated as conversion anodes in lithium half-cells and delivered significantly higher capacities than two-component MgFe<sub>2</sub>O<sub>4</sub> made by combustion synthesis. X-ray absorption near-edge structure (XANES) was used to estimate the oxidation states of the metals in the pristine, lithiated (discharged) and delithiated (charged) materials to better understand the redox processes in half cells that led to the improvement. Co, Ni, and Zn are reduced to low oxidation states during lithiation (cell discharge) but are only partially oxidized. The presence of a conductive metallic network that forms after lithiation is thought to account for the improved electrochemical characteristics. Interestingly, in most of the samples, iron is not fully reduced during initial lithiation unlike what happens with a set of related high entropy spinel ferrites studied previously. The improved electrochemical properties of these materials illustrates both the advantages of complexity and the difficulties in predicting their behavior.

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Publication Details

Journal
ACS Applied Materials & Interfaces
Published
2025-04-07
DOI
https://doi.org/10.1021/acsami.4c21332
Citations
4
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
2.92
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Compositionally Complex Spinel Oxides as Conversion Anodes for Lithium-Ion Batteries

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ACS Applied Materials & Interfaces
Advancements in Battery Materials
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article

Compositionally Complex Spinel Oxides as Conversion Anodes for Lithium-Ion Batteries

Juhyeon Ahn, Lu Ma, Amy C. Marschilok, Mary Scott, Jianming Bai, A. Pace, Kenneth J. Takeuchi, Ki-Hun Nam, Zachary R. Mansley, Seung‐Kyu Kim, Esther S. Takeuchi, Zhongling Wang, Marca M. Doeff, Marie F. Millares, Shan Yan, Myoung Hwan Oh, Cynthia Huang, Steven N. Ehrlich, Armando Rodriguez-Campos, Yimei Zhu, Jessica Luo
article en
4 citations

Abstract

Four different compositionally complex multicomponent M<sub>3</sub>O<sub>4</sub> spinels containing 5-8 distinct metals were prepared by a rapid combustion synthesis method or solvothermal synthesis. High resolution synchrotron X-ray diffraction patterns show that the materials consist primarily of spinel phases with small amounts of rock salt impurities, and, in several samples, a minor amount of contracted spinel phase. Materials were investigated as conversion anodes in lithium half-cells and delivered significantly higher capacities than two-component MgFe<sub>2</sub>O<sub>4</sub> made by combustion synthesis. X-ray absorption near-edge structure (XANES) was used to estimate the oxidation states of the metals in the pristine, lithiated (discharged) and delithiated (charged) materials to better understand the redox processes in half cells that led to the improvement. Co, Ni, and Zn are reduced to low oxidation states during lithiation (cell discharge) but are only partially oxidized. The presence of a conductive metallic network that forms after lithiation is thought to account for the improved electrochemical characteristics. Interestingly, in most of the samples, iron is not fully reduced during initial lithiation unlike what happens with a set of related high entropy spinel ferrites studied previously. The improved electrochemical properties of these materials illustrates both the advantages of complexity and the difficulties in predicting their behavior.

ACS Applied Materials & InterfacesVol. 17(15)
Lawrence Berkeley National Laboratory (US), Brookhaven National Laboratory (US), Sustainability Institute (ZA), Stanford Synchrotron Radiation Lightsource (US), Korea Institute of Energy Research (KR), Foundry (United Kingdom) (GB), Molecular Foundry, National Synchrotron Light Source II, Stony Brook University (US), University of California, Berkeley (US)
Affordable and clean energy
Openalex Percentile: Top 10%
Advancements in Battery Materials
2.92
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