The increasing demand for Li-ion batteries across various energy storage applications underscores the urgent need for environmentally friendly and efficient direct recycling strategies to address the issue of substantial cathode waste. Diverse reducing agents for Li supplements, such as quinone molecules, have been considered to homogenize the Li distribution in the cathode materials obtained after cycling; however, the detailed reaction mechanism is still unknown. Herein, the ideal electrochemical potential factor and reaction mechanism of the redox mediator 3,5-di-tert-butyl-o-benzoquinone (DTBQ) for the chemical relithiation of high-Ni-layered cathodes are elucidated. Here, 100% efficiency of DTBQ-assisted chemical relithiation is achieved by adjusting the direct immersion time of Li-deficient cathode electrodes. The reversible reaction features of the physical and chemical structures of both the regenerated cathodes and the DTBQ molecules are investigated using advanced characterization and density functional theory calculations. These findings emphasize the potential of redox-mediator-assisted chemical relithiation for realizing direct recycling processes and offer a facile and sustainable solution for battery recycling.
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http://dx.doi.org/10.1002/advs.202417094 | DOI Listing |
Adv Sci (Weinh)
January 2025
Department of Chemical and Biological Engineering, Sookmyung Women's University, 100 Cheongpa-ro 47-gil, Yongsan-gu, Seoul, 04310, Republic of Korea.
The increasing demand for Li-ion batteries across various energy storage applications underscores the urgent need for environmentally friendly and efficient direct recycling strategies to address the issue of substantial cathode waste. Diverse reducing agents for Li supplements, such as quinone molecules, have been considered to homogenize the Li distribution in the cathode materials obtained after cycling; however, the detailed reaction mechanism is still unknown. Herein, the ideal electrochemical potential factor and reaction mechanism of the redox mediator 3,5-di-tert-butyl-o-benzoquinone (DTBQ) for the chemical relithiation of high-Ni-layered cathodes are elucidated.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
China-UK Low Carbon College, Shanghai Jiao Tong University, Shanghai 200240, China.
Direct regeneration, which involves replenishing lithium in spent cathode materials, is emerging as a promising recycling technique for spent lithium iron phosphate (s-LFP) cathodes. Unlike solid-state regeneration, the aqueous relithiation method consumes less energy, ensures even lithium replenishment, and significantly recovers the capacity of s-LFP. However, liquid-phase lithium replenishment formulations are generally less standardized.
View Article and Find Full Text PDFNat Commun
November 2024
Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California, San Diego, La Jolla, CA, 92093, USA.
LiNiCoMnO (0 < x, y < 1, NCM) is the dominant positive material for the state-of-the-art lithium-ion batteries. However, the sensitivity of NCM materials to moisture makes their manufacturing, storage, transportation, electrode processing and recycling complicated. Although it is recognized that protons play a critical role in their structure stability and performance, proton exchange with Li in NCM materials has not been well understood.
View Article and Find Full Text PDFACS Nano
November 2024
Program of Materials Science and Engineering, University of California San Diego, La Jolla, California 92093, United States.
Despite significant progress in recycling spent lithium-ion batteries (LIBs), nondestructive, direct recycling methods still face untenable discrepancies in multiple cathode chemistries, which primarily originate from a variety of structure stabilities during the recycling process. Through systematic investigation of the microstructure evolution during the relithiation treatment, we observed the inevitably induced defects and Li/Mn disordering in the LiNiMnO cathode, contributing to the sluggish Li transport and irreversible capacity loss. Employing a defect engineering approach to achieve twin boundaries and preferred grain orientation, we show the regenerated cathodes demonstrate a substantial enhancement of Li diffusion and cycling stability, retaining 97.
View Article and Find Full Text PDFInorg Chem
September 2024
College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China.
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