Probing Hybrid LiFePO4/FePO4 Phases in a Single Olive LiFePO4 Particle and Their Recovering from Degraded Electric Vehicle Batteries

Wenyu Wang; Rui Wang; Renming Zhan; Junmou Du; Zihe Chen; Ruikang Feng; Yuchen Tan; Yang Hu; Yangtao Ou; Yifei Yuan; Cheng Li; Yinguo Xiao; Yongming Sun

doi:10.1021/acs.nanolett.3c01991

Probing Hybrid LiFePO₄/FePO₄ Phases in a Single Olive LiFePO₄ Particle and Their Recovering from Degraded Electric Vehicle Batteries

Wenyu Wang, Rui Wang, Renming Zhan, Junmou Du, Zihe Chen, Ruikang Feng, Yuchen Tan, Yang Hu, Yangtao Ou, Yifei Yuan, Cheng Li, Yinguo Xiao, Yongming Sun

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Research output: Contribution to journal › Article › peer-review

12 Scopus citations

Abstract

The recycling of LiFePO₄ from degraded lithium-ion batteries (LIBs) from electric vehicles (EVs) has gained significant attention due to resource, environment, and cost considerations. Through neutron diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy, we revealed continuous lithium loss during battery cycling, resulting in a Li-deficient state (Li_1-xFePO₄) and phase separation within individual particles, where olive-shaped FePO₄ nanodomains (5-10 nm) were embedded in the LiFePO₄ matrix. The preservation of the olive-shaped skeleton during Li loss and phase change enabled materials recovery. By chemical compensation for the lithium loss, we successfully restored the hybrid LiFePO₄/FePO₄ structure to pure LiFePO₄, eliminating nanograin boundaries. The regenerated LiFePO₄ (R-LiFePO₄) exhibited a high crystallinity similar to the fresh counterpart. This study highlights the importance of topotactic chemical reactions in structural repair and offers insights into the potential of targeted Li compensation for energy-efficient recycling of battery electrode materials with polyanion-type skeletons.

Original language	English
Pages (from-to)	7485-7492
Number of pages	8
Journal	Nano Letters
Volume	23
Issue number	16
DOIs	https://doi.org/10.1021/acs.nanolett.3c01991
State	Published - Aug 23 2023

Funding

This work is financially supported by the Natural Science Foundation of China (Grant No. 52072137, No. 52272207, and No. 52072888) and Innovation Fund of Wuhan National Laboratory for Optoelectronics of Huazhong University of Science and Technology. The authors would like to thank the Analytical and Testing Center of Huazhong University of Science and Technology. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory.

Funders	Funder number
Office of Science
Oak Ridge National Laboratory
National Natural Science Foundation of China	52072888, 52072137, 52272207
Huazhong University of Science and Technology

Keywords

degraded lithium-ion batteries
hybrid LiFePO/FePO
regeneration
single particle
targeted Li compensation

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1021/acs.nanolett.3c01991

Cite this

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title = "Probing Hybrid LiFePO4/FePO4 Phases in a Single Olive LiFePO4 Particle and Their Recovering from Degraded Electric Vehicle Batteries",

abstract = "The recycling of LiFePO4 from degraded lithium-ion batteries (LIBs) from electric vehicles (EVs) has gained significant attention due to resource, environment, and cost considerations. Through neutron diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy, we revealed continuous lithium loss during battery cycling, resulting in a Li-deficient state (Li1-xFePO4) and phase separation within individual particles, where olive-shaped FePO4 nanodomains (5-10 nm) were embedded in the LiFePO4 matrix. The preservation of the olive-shaped skeleton during Li loss and phase change enabled materials recovery. By chemical compensation for the lithium loss, we successfully restored the hybrid LiFePO4/FePO4 structure to pure LiFePO4, eliminating nanograin boundaries. The regenerated LiFePO4 (R-LiFePO4) exhibited a high crystallinity similar to the fresh counterpart. This study highlights the importance of topotactic chemical reactions in structural repair and offers insights into the potential of targeted Li compensation for energy-efficient recycling of battery electrode materials with polyanion-type skeletons.",

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author = "Wenyu Wang and Rui Wang and Renming Zhan and Junmou Du and Zihe Chen and Ruikang Feng and Yuchen Tan and Yang Hu and Yangtao Ou and Yifei Yuan and Cheng Li and Yinguo Xiao and Yongming Sun",

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AU - Wang, Wenyu

AU - Wang, Rui

AU - Zhan, Renming

AU - Du, Junmou

AU - Chen, Zihe

AU - Feng, Ruikang

AU - Tan, Yuchen

AU - Hu, Yang

AU - Ou, Yangtao

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AU - Xiao, Yinguo

AU - Sun, Yongming

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N2 - The recycling of LiFePO4 from degraded lithium-ion batteries (LIBs) from electric vehicles (EVs) has gained significant attention due to resource, environment, and cost considerations. Through neutron diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy, we revealed continuous lithium loss during battery cycling, resulting in a Li-deficient state (Li1-xFePO4) and phase separation within individual particles, where olive-shaped FePO4 nanodomains (5-10 nm) were embedded in the LiFePO4 matrix. The preservation of the olive-shaped skeleton during Li loss and phase change enabled materials recovery. By chemical compensation for the lithium loss, we successfully restored the hybrid LiFePO4/FePO4 structure to pure LiFePO4, eliminating nanograin boundaries. The regenerated LiFePO4 (R-LiFePO4) exhibited a high crystallinity similar to the fresh counterpart. This study highlights the importance of topotactic chemical reactions in structural repair and offers insights into the potential of targeted Li compensation for energy-efficient recycling of battery electrode materials with polyanion-type skeletons.

AB - The recycling of LiFePO4 from degraded lithium-ion batteries (LIBs) from electric vehicles (EVs) has gained significant attention due to resource, environment, and cost considerations. Through neutron diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy, we revealed continuous lithium loss during battery cycling, resulting in a Li-deficient state (Li1-xFePO4) and phase separation within individual particles, where olive-shaped FePO4 nanodomains (5-10 nm) were embedded in the LiFePO4 matrix. The preservation of the olive-shaped skeleton during Li loss and phase change enabled materials recovery. By chemical compensation for the lithium loss, we successfully restored the hybrid LiFePO4/FePO4 structure to pure LiFePO4, eliminating nanograin boundaries. The regenerated LiFePO4 (R-LiFePO4) exhibited a high crystallinity similar to the fresh counterpart. This study highlights the importance of topotactic chemical reactions in structural repair and offers insights into the potential of targeted Li compensation for energy-efficient recycling of battery electrode materials with polyanion-type skeletons.

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