Abstract
Electrochemical intercalation offers a promising platform for Li+ extraction. However, only limited types of electrode materials have been investigated. The challenge to broaden and tailor materials for electrochemical intercalation-based Li+ extraction lies in the lack of understanding of material’s response upon co-intercalation of multiple ions, therefore, paired process design to enable reversible Li+ extraction and recovery. Here, we showcase the design of asymmetric ion pathways for Li+ extraction and recovery for host material with complex Li+ and Na+ interaction using layered cobalt oxide as a model material. The two-phase equilibrium of Na0.48CoO2 and Li0.94CoO2 governs Li+ selectivity when a high depth of intercalation is achieved (low vacancy level). We show that the relative rate between ion exchange and intercalation is critical to determine the ion pathways. The relationship can be quantitatively compared using the average pseudo ion exchange rate (CpseudoIX) and the intercalation rate (Cinter). The ion pathways at the three regimes with CpseudoIX > Cinter, CpseudoIX ~ Cinter, and CpseudoIX <Cinter are constructed. By selecting the optimized ion pathway and particle size, we demonstrate 9.7×104 Li+ selectivity with 99% purity Li+ recovery from an initial 1:1000 Li: Na molar ratio solution using 115 mAh/g specific capacity.
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Acknowledgements
We give acknowledgments to Joanna E. Stubbs and Peter J. Eng for helping with the in situ XRD setup. This work made use of instruments in the Electron Microscopy Core of UIC’s Research Resources Center. This work is supported by the US Department of Energy (DOE), Office of Basic Energy Sciences under award DE-SC0022984. C. L. acknowledges the support from the Camille Dreyfus Teacher-Scholar Award TC-23-041. This work used instruments from the University of Chicago Materials Research Science and Engineering Center, funded by the National Science Foundation (NSF) under award number DMR-2011854. Portions of this work were performed at GeoSoilEnviroCARS (The University of Chicago, Sector 13), Advanced Photon Source (APS), Argonne National Laboratory. GeoSoilEnviroCARS was supported by the National Science Foundation – Earth Sciences (EAR – 1634415). This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Sciences, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515.
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Hill, G.T., Stone, R., Han, Y. et al. Asymmetric pathways for lithium extraction and recovery based on the two-phase equilibrium of layered oxides. Nat Commun (2026). https://doi.org/10.1038/s41467-026-72755-4
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DOI: https://doi.org/10.1038/s41467-026-72755-4
