Compensating the irreversible loss of limited active lithium (Li) is essentially important for improving the energy-density and cycle-life of practical Li-ion battery full-cell, especially after employing high-capacity but low initial coulombic efficiency anode candidates. Introducing prelithiation agent can provide additional Li source for such compensation. Herein, we precisely implant trace Co (extracted from transition metal oxide) into the Li site of Li O, obtaining (Li Co □ ) O (CLO) cathode prelithiation agent. The synergistic formation of Li vacancies and Co-derived catalysis efficiently enhance the inherent conductivity and weaken the Li-O interaction of Li O, which facilitates its anionic oxidation to peroxo/superoxo species and gaseous O , achieving 1642.7 mAh/g prelithiation capacity (≈980 mAh/g for prelithiation agent). Coupled 6.5 wt % CLO-based prelithiation agent with LiCoO cathode, substantial additional Li source stored within CLO is efficiently released to compensate the Li consumption on the SiO/C anode, achieving 270 Wh/kg pouch-type full-cell with 92 % capacity retention after 1000 cycles.
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http://dx.doi.org/10.1002/anie.202316112 | DOI Listing |
ACS Appl Mater Interfaces
November 2024
Centre for Cooperative Research on Alternative Energies (CIC energiGUNE), Basque Research and Technology Alliance (BRTA), Alava Technology Park, Albert Einstein 48, 01510 Vitoria-Gasteiz, Spain.
Prelithiation is a critical step in dual carbon lithium-ion capacitors (LICs) due to the lack of Li in the system, which needs to be incorporated externally to avoid electrolyte depletion. Several prelithiation techniques have been developed over the years, and recently, dilithium squarate (LiCO) has been reported as an air-stable, easy to synthesize, safe, and cost-effective prelithiation reagent for LICs. LiCO has successfully been used in a wide range of chemistries, and its integration into positive electrodes has been scaled up to roll-to-roll processing and demonstrated in multilayer pouch cells.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, and Frontiers Science, Center for Critical Earth Material Cycling, Nanjing University, Nanjing, 210023, China.
Adv Mater
November 2024
State Key Laboratory of Solidification Processing, Centre for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi'an, 710072, China.
The substantial manufacturing of lithium-ion batteries (LIBs) requires sustainable, circular, and decarbonized recycling strategies. While efforts are concentrated on extracting valuable metals from cathodes using intricate chemical process, the direct, efficient cathode regeneration remains a technological challenge. More urgently, the battery supply chain also requires the value-added exploitation of retired anodes.
View Article and Find Full Text PDFMolecules
June 2024
College of Energy, Xiamen University, Xiamen 361102, China.
In conventional lithium-ion batteries (LIBs), the active lithium from the lithium-containing cathode is consumed by the formation of a solid electrolyte interface (SEI) at the anode during the first charge, resulting in irreversible capacity loss. Prelithiation additives can provide additional active lithium to effectively compensate for lithium loss. Lithium oxalate is regarded as a promising ideal cathode prelithiation agent; however, the electrochemical decomposition of lithium oxalate is challenging.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
August 2024
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Centre for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.
The surge in lithium-ion batteries has heightened concerns regarding metal resource depletion and the environmental impact of spent batteries. Battery recycling has become paramount globally, but conventional techniques, while effective at extracting transition metals like cobalt and nickel from cathodes, often overlook widely used spent LiFePO due to its abundant and low-cost iron content. Direct regeneration, a promising approach for restoring deteriorated cathodes, is hindered by practicality and cost issues despite successful methods like solid-state sintering.
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