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Amidst global sustainability imperatives, this study pioneers a solid-state regeneration strategy that transforms spent LiCoO (LCO) cathodes into high-performance materials via amorphous lithium iron phosphate glass (LFPg)-driven structural reconfiguration. Unlike conventional recycling that decomposes cathodes, our approach leverages LFPg's defect-rich framework, high ionic conductivity, and dynamic interfacial activity to directly reconstruct degraded LCO crystals. The LFPg acts as a multifunctional repair agent: creating Li diffusion channels through disorder engineering, eliminating oxygen vacancies via atomic oxygen transfer, scavenging impurities (e.g., F-, C-F), and homogenizing Co/Co redox states. Regenerated cathodes (LCO:LFPg = 8:2) achieve a record 214.6 mAh/g at 0.5C─surpassing commercial LCO─and retain 86.1% capacity after 100 cycles (163.9 mAh/g) with near-100% Coulombic efficiency, while charge-transfer resistance plummets 78.2%. This energy-efficient, atom-economic process establishes a paradigm for battery circularity, positioning amorphous-phase engineering as the key to sustainable high-value resource recovery.
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http://dx.doi.org/10.1021/acs.langmuir.5c03201 | DOI Listing |
ACS Appl Mater Interfaces
September 2025
Department of Agricultural and Biosystems Engineering, South Dakota State University, Brookings, South Dakota 57007, United States.
Metal-organic frameworks (MOFs)/polymer composite electrolytes have garnered worldwide attention because of their outstanding performance in energy-related applications. Here, a highly lithiated MOF (LZM) is designed as a filler into poly(ethylene oxide) (PEO). LZM is synthesized through a postsynthetic modified strategy to obtain preeminent single-ion conducting performance.
View Article and Find Full Text PDFLangmuir
September 2025
School of Materials Science and Engineering, Changchun University of Science and Technology, Changchun, Jilin 130022, P.R. China.
Amidst global sustainability imperatives, this study pioneers a solid-state regeneration strategy that transforms spent LiCoO (LCO) cathodes into high-performance materials via amorphous lithium iron phosphate glass (LFPg)-driven structural reconfiguration. Unlike conventional recycling that decomposes cathodes, our approach leverages LFPg's defect-rich framework, high ionic conductivity, and dynamic interfacial activity to directly reconstruct degraded LCO crystals. The LFPg acts as a multifunctional repair agent: creating Li diffusion channels through disorder engineering, eliminating oxygen vacancies via atomic oxygen transfer, scavenging impurities (e.
View Article and Find Full Text PDFJ Mater Chem A Mater
August 2025
Institute for Theoretical Physics, University of Amsterdam Science Park 904 Amsterdam 1098 XH The Netherlands
The quest for high-capacity anode materials is vital in developing future lithium-ion battery technologies. While silicon-based anodes offer high theoretical capacity, their commercial realization is hindered by instability associated with large volume changes. Amorphous silicon nitride (a-SiN) has emerged as a promising alternative, acting as a conversion-type anode where lithium incorporation drives the formation of a structurally robust matrix and active phases.
View Article and Find Full Text PDFJ Am Chem Soc
August 2025
Eastern Institute for Advanced Study, Ningbo Institute of Digital Twin, Eastern Institute of Technology, Zhejiang Key Laboratory of All-Solid-State Battery, Ningbo Key Laboratory of All-Solid-State Battery Eastern Institute of Technology, Ningbo, Zhejiang 315200, P.R. China.
Lithium sulfide (LiS), a key cathode material for all-solid-state lithium-sulfur (Li-S) batteries, faces challenges such as low electronic and ionic conductivities and limited active material utilization during cycling. In this study, we developed a new cathode featuring nanosized LiS embedded in an amorphous LiFeS matrix (92LiS@8LiFeS). Benefiting from the mixed electronic and ionic conductivities of LiFeS along with its catalytic effect and the nanosized LiS that shortens electron and ion transport distances, this 92LiS@8LiFeS cathode exhibits long-term cycling stability with a capacity retention of over 99% after 320 cycles.
View Article and Find Full Text PDFAdv Mater
August 2025
Division of Energy Storage, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
Halide cathode active materials (CAMs) with high ionic conductivities have attracted significant attention. However, their capacity and energy density are limited by the large molar weight of the Li⁺ transport-dependent MCl anionic framework. In this study, a low-cost amorphous iron-based oxyhalide LFFOC-0.
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