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Low-cost iron trichloride cathode for all-solid-state lithium-ion batteries

Nature Sustainability (2024)Cite this article

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Abstract

The dominant chemistries of lithium-ion batteries on the market today still rely on flammable organic liquid electrolytes and cathodes containing scarce metals, such as cobalt or nickel, raising safety, cost and environmental concerns. Here we show a FeCl3 cathode that costs as little as 1% of the cost of a LiCoO2 cathode or 2% of a LiFePO4 cathode. Once coupled with a solid halide electrolyte and a lithium-indium (Li–In) alloy anode, it enables all-solid-state lithium-ion batteries without any liquid components. Notably, FeCl3 exhibits two flat voltage plateaux between 3.5 and 3.8 V versus Li+/Li, and the solid cell retains 83% of its initial capacity after 1,000 cycles with an average Coulombic efficiency of 99.95%. Combined neutron diffraction and X-ray absorption spectroscopy characterizations reveal a Li-ion (de)intercalation mechanism together with a Fe2+/Fe3+ redox process. Our work provides a promising avenue for developing sustainable battery technologies with a favourable balance of performance, cost and safety.

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Fig. 1: Crystal structure of FeCl3.
Fig. 2: Electrochemical performance of FeCl3 in solid cells.
Fig. 3: Redox-active element in FeCl3 in the charging and discharging processes.
Fig. 4: Structural characterization.
Fig. 5: Energy density and cost.

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All data in this work are available in the text and Supplementary Information. Source data are provided with this paper.

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Acknowledgements

Z.L. and H.C. acknowledge financial support from the National Science Foundation (Grant Nos. 1706723 and 2108688) and from the faculty startup fund of Georgia Tech. The Advanced Photon Source at Argonne National Laboratory was made available through the General User Program, which is supported by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (Contract No. DE-AC02-06CH11357). This research also used the 28ID-2 XPD beamline of the National Synchrotron Light Source II, a DOE, Office of Science user facility operated for the DOE Office of Science by Brookhaven National Laboratory (Contract No. DE-SC0012704). A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science user facility operated by Oak Ridge National Laboratory. J.L. thanks the DOE, Office of Science, Office of Basic Energy Sciences for funding support (Grant No. DOE-BES-ERKCSNX). S.Z. and Y.T. acknowledge support from the National Science Foundation (Grant No. 1923802) and NASA (Grant No. 80NSSC21K0483). We thank the beamline scientists J. Okasinski, J. Bai and W. Xu for their help with the synchrotron experiments. We thank Z. Fan’s group at the University of Houston for assisting with scanning electron microscopy characterizations.

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Author notes

  1. These authors contributed equally: Zhantao Liu, Jue Liu.

Authors and Affiliations

  1. George W. Woodruff School of Mechanical Engineering, Georgia Institute of Technology, Atlanta, GA, USA

    Zhantao Liu, Ting Zhu & Hailong Chen

  2. Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN, USA

    Jue Liu

  3. School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA

    Simin Zhao & Yuanzhi Tang

  4. School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, GA, USA

    Sangni Xun

  5. Department of Physics, University of Houston, Houston, TX, USA

    Paul Byaruhanga & Shuo Chen

  6. Texas Center for Superconductivity, University of Houston, Houston, TX, USA

    Paul Byaruhanga & Shuo Chen

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Contributions

Z.L. and H.C. conceived the ideas and designed the experiments. Z.L conducted the synthesis, electrochemical testing and part of the characterizations. J.L. S.Z., S.X., P.B., S.C. and Y.T. contributed to the characterization of materials. J.L. contributed to the structure analysis and wrote part of the manuscript. Z.L., T.Z. and H.C. wrote the manuscript. All authors reviewed and revised the manuscript.

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Correspondence to Hailong Chen.

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Competing interests

Z.L. and H.C. have filed a US provisional patent application (63/363,875) covering the application of FeCl3 and related compounds as cathode materials in solid-state batteries as described in this paper. The remaining authors declare no competing interests.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–22 and Tables 1–7.

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Source data

Source Data Fig. 1

Rietveld refinement results of synchrotron XRD for pristine FeCl3.

Source Data Fig. 2

Electrochemical performance of FeCl3 in solid cells.

Source Data Fig. 3

XANES results of FeCl3 at different discharge and charge stages.

Source Data Fig. 4

Operando EDXRD results of the FeCl3 solid cell and Rietveld refinement results of Li0.8FeCl3.

Source Data Fig. 5

Comparison of costs between FeCl3 and other cathode materials.

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Liu, Z., Liu, J., Zhao, S. et al. Low-cost iron trichloride cathode for all-solid-state lithium-ion batteries. Nat Sustain (2024). https://doi.org/10.1038/s41893-024-01431-6

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