4.6 Article

Pitch Carbon-coated Ultrasmall Si Nanoparticle Lithium-ion Battery Anodes Exhibiting Reduced Reactivity with Carbonate-based Electrolyte

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BATTERIES & SUPERCAPS
卷 6, 期 9, 页码 -

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WILEY-V C H VERLAG GMBH
DOI: 10.1002/batt.202300186

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silicon nanoparticle anodes; pitch carbon-coating; lithium-ion batteries; carbonate-based electrolytes; high loading full-cells

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Silicon anodes have high energy density potential but suffer from poor lifetimes due to mechanical and chemical reactivity issues. This study presents a pitch carbon-coated silicon composite anode that reduces reactivity with carbonate-based electrolytes. By minimizing particle size and employing conformal coatings, the anode retains 75% capacity after 1000 cycles when paired with a high voltage cathode. However, increasing energy density leads to severe mechanical degradation, posing a challenge for future work.
Silicon anodes for lithium-ion batteries (LIBs) have the potential for higher energy density compared to conventionally used graphite-based LIB anodes. However, silicon anodes exhibit poor cycle and calendar lifetimes due to mechanical instabilities and high chemical and electrochemical reactivity with the carbonate-based electrolytes that are typically used in LIBs. In this work, we synthesize a pitch carbon-coated silicon nanoparticle composite active material for LIB anodes that exhibits reduced chemical reactivity with carbonate-based electrolytes compared to an uncoated silicon anode. Silicon primary particle sizes less than 10 nm diameter minimize micro-scale mechanical degradation of the anode composite, while conformal coatings of pitch carbon minimize the parasitic reactions between the silicon and the electrolyte. When matched with a high voltage NMC622 (LiNi0.6Mn0.2Co0.2O2) cathode, the pitch carbon-coated silicon anode retains & AP;75 % of its initial capacity at the end of 1000 cycles. Increasing the areal loading of the pitch carbon-coated silicon anodes to realize energy density improvements over graphite anodes results in severe mechanical degradation on the electrode level, highlighting a remaining challenge to be addressed in future work.

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