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DOE OSTI · 3008063

In Situ Surface Reconstruction via Lithium Residue Regulation for Direct Recycling of Ni-Rich Cathodes

Lin, Jiao [Univ. of California, San Diego, CA (United States)]·Gupta, Varun [Univ. of California, San Diego, CA (United States)] (ORCID:0000000249768593)·Yu, Xiaolu [Univ. of California, San Diego, CA (United States)]·Zhu, Yuwei [Arizona State Univ., Tempe, AZ (United States)]·Lee, Dong Ju [Univ. of California, San Diego, CA (United States)] (ORCID:0000000285834957)·Zhao, Zishuo [Arizona State Univ., Tempe, AZ (United States)]·Xiao, Xianghui [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000271423452)·Feagure, Greta [Univ. of California, San Diego, CA (United States)]·Li, Feng [Univ. of California, San Diego, CA (United States)] (ORCID:0000000306200639)·Gao, Hongpeng [Univ. of California, San Diego, CA (United States)] (ORCID:0000000266404070)·Nordlund, Dennis [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)]·Mu, Linqin [Arizona State Univ., Tempe, AZ (United States)] (ORCID:0000000344214820)·Chen, Zheng [Univ. of California, San Diego, CA (United States)] (ORCID:0000000291864298)
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Abstract

Surface stability is crucial for the long cycling performance of Ni-rich cathodes, as it dictates and governs side reactions, preserves crystal integrity, and mitigates capacity degradation during cycling. For spent Ni-rich cathodes targeted for one-step direct recycling, constructing a robust and stable surface is particularly challenging because prior cycling induces severe structural and morphological degradation. Here, in this study, we introduce an in situ surface reconstruction strategy that converts surface lithium residues into a protective layer via a direct liquid-phase coating with ammonium dihydrogen phosphate (ADP). During the process, residual lithium remaining after the hydrothermal relithiation is removed, while a conformal lithium phosphate (Li 3 PO 4 , LPO) layer is formed to act as both a chemical barrier and a structural stabilizer. This dual function enhances cycling stability and rate capability in regenerated cathodes, and the approach is applicable to various Ni-rich compositions including spent LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622) and scrap LiNi 0.866 Mn 0.066 Co 0.05 Al 0.018 O 2 (NCMA). Its scalability and compositional versatility make it a promising route for sustainable regeneration of high-performance cathode materials.

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36 MATERIALS SCIENCENi-rich cathodesdirect recyclingin situ surface reconstructionlithium phosphate layerspent lithium-ion batteries

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Lin, Jiao [Univ. of California, San Diego, CA (United States)], Gupta, Varun [Univ. of California, San Diego, CA (United States)] (ORCID:0000000249768593), Yu, Xiaolu [Univ. of California, San Diego, CA (United States)], Zhu, Yuwei [Arizona State Univ., Tempe, AZ (United States)], Lee, Dong Ju [Univ. of California, San Diego, CA (United States)] (ORCID:0000000285834957), Zhao, Zishuo [Arizona State Univ., Tempe, AZ (United States)], Xiao, Xianghui [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000271423452), Feagure, Greta [Univ. of California, San Diego, CA (United States)], Li, Feng [Univ. of California, San Diego, CA (United States)] (ORCID:0000000306200639), Gao, Hongpeng [Univ. of California, San Diego, CA (United States)] (ORCID:0000000266404070), Nordlund, Dennis [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)], Mu, Linqin [Arizona State Univ., Tempe, AZ (United States)] (ORCID:0000000344214820), Chen, Zheng [Univ. of California, San Diego, CA (United States)] (ORCID:0000000291864298). 2025-11-19. In Situ Surface Reconstruction via Lithium Residue Regulation for Direct Recycling of Ni-Rich Cathodes. https://doi.org/10.1021/acsnano.5c13656

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The transition to a flexible and reliable energy infrastructure, using electro-thermal energy generation technologies such as geothermal, concentrated solar power, and nuclear, usually demands simultaneous advancement of thermal energy storage (TES) to support on-demand electricity generation and industrial applications while mitigating the inherent intermittency of renewable energy sources and power outages from direct energy generation. Among TES technologies, thermochemical energy storage (TCES) based on calcium looping emerges as a compelling high-power energy storage candidate due to its high reaction enthalpy, compatibility with elevated operating temperatures, and abundance of low-cost materials. However, the long-term durability of calcium-based sorbents for TCES is hindered by surface sintering and particle aggregation, leading to performance degradation over repeated thermal cycles. This study explores a moisture hydration-based strategy to regenerate a degraded calcium sorbent and mitigate performance degradation for long duration TCES. The addition of moisture transforms calcium oxide into calcium hydroxide and produces intercalation water layers, associated with a regenerated surface area and reduced calcium oxide crystallite size. Both these effects are beneficial in restoring the sorbents' reactivity for carbonization. Additionally, an optimized hydration-assisted reactivation protocol balances the recovered energy storage capacity with heating penalty required for moisture removal from hydrated samples, resulting in an enhanced energy storage capacity up to 176% compared to benchmark sorbents that undergo cycling without reactivation after 60 cycles. In conclusion, these results highlight the potential of hydration-assisted reactivation to enhance the long-term performance of TCES, providing an effective pathway to advancing electro-thermal storage technologies.

36 MATERIALS SCIENCE↗