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Chemical prelithiation is an effective method to compensate for the loss of active lithium due to the formation of solid electrolyte interface, effectively addressing the issue of low initial coulombic efficiency (ICE) in silicon/carbon (Si/C) materials. Herein, the Si/C anode is prelithiated in a 1 M lithium-phenanthrene/2-methyltetrahydrofuran (Li-Phe/2-MTHF) solution in our work, and the prelithiated Si/C anode is followed by post-treatment with commercial electrolytes containing lithium difluorobis(oxalato)phosphate (LiDFBOP). The PSi/C-L, originated from the reaction between residual Li-Phe/2-MTHF and the commercial electrolyte containing 0.5 wt% LiDFBOP, possesses the artificial SEI film, which not only contains a proper amount of LiF but also is rich in LiCO and LiP. Among them, LiF and LiCO ensures the stability of the SEI film. Simultaneously, the synergistic effect of LiP and LiF improves its Li transport kinetics. Therefore, the ICE of PSi/C-L reaches 92.50 %, and almost no drop in capacity occurs after 100 cycles at 0.5 A/g. Furthermore, the capacity stays steady at about 270 mAh/g through nearly 500 cycles at 1 A/g, achieving an impressive capacity retention rate of 97.8 %, significantly outperforming un-treated Si/C. This study offers new directions for constructing SEI films with stable structures and high Li kinetics transport.
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http://dx.doi.org/10.1016/j.jcis.2025.02.136 | DOI Listing |
Adv Mater
August 2025
State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
To improve the energy density of Li-ion batteries, conventional sacrificial prelithiation agents (LiFeO, LiO and LiCO, etc.) are introduced to compensate for active lithium loss, but they undergo serious volumetric shrinkage during decomposition, generating voids that compromise electrode architecture integrity and deteriorate electrochemical performance. Herein, the typical Li-rich layered oxide cathode is converted into Li-rich disordered rocksalt oxide (LRDO) prelithiation agent, achieving 330 mAh g charge capacity and retaining 130 mAh g reversible capacity (contributing 200 mAh g irreversible prelithiation capacity).
View Article and Find Full Text PDFAdv Mater
August 2025
George W. Woodruff School of Mechanical Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
Solid-state batteries with alloy-type negative electrodes can feature enhanced energy density and safety compared to conventional Li-ion batteries. However, diffusional Li trapping within Li alloys often causes low initial Coulombic efficiency and leads to capacity loss with cycling. Here, a general roll-pressing prelithiation method compatible with a variety of alloy-type negative electrodes (silicon, aluminum, tin, and multi-phase alloys) is introduced, which is shown to improve performance in solid-state batteries.
View Article and Find Full Text PDFChemistry
August 2025
Inorganic Chemistry, TU Dortmund University, Otto-Hahn-Str. 6, 44227, Dortmund, Germany.
Deprotonation reactions with lithium alkyls exhibit a high temperature dependency. However, the reactivity of lithium alkyls with conventionally used Lewis bases limits their deprotonation capability of more challenging substrates like tertiary amines. Therefore, we have focused on the use of high but exactly set reaction temperatures by usage of microwave radiation in the deprotonation reaction of a tertiary amine in the absence of polar additives.
View Article and Find Full Text PDFJ Am Chem Soc
August 2025
Hubei Key Laboratory of Electrochemical Power Sources, College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, Hubei 430072, China.
Developing lithium-enriched cathodes, such as LiNCM523 ( ≥ 0), offers a promising approach to boost the cycling life of anode-free lithium metal batteries (AFLMBs). However, the traditional electrochemical prelithiation method is confined to laboratory studies, while conventional chemical prelithiation using highly reductive reagents like biphenyllithium (0.25 V vs Li/Li) often causes severe surficial excessive-lithiation and structural degradation, compromising battery performance.
View Article and Find Full Text PDFNatl Sci Rev
July 2025
School of Chemistry, South China Normal University, Guangzhou 510006, China.
Improving the initial Coulombic efficiency (ICE) of silicon anodes in lithium-ion batteries is a key challenge for enhancing their performance. Traditional prelithiation methods, such as using lithium naphthalenide (Li-Naph), are limited by the low lithiation potential of crystalline silicon, making them less effective for commercial applications. This study demonstrates that amorphous silicon anodes, with a higher lithiation potential, can be effectively prelithiated using Li-Naph.
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