Pitch Carbon-Coated Ultrasmall Si Nanoparticle Lithium-Ion Battery Anodes Exhibiting Reduced Reactivity with Carbonate-Based Electrolyte

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Abstract

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 ≈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.

Original languageAmerican English
Article numbere202300186
Number of pages8
JournalBatteries and Supercaps
Volume6
Issue number9
DOIs
StatePublished - 2023

Bibliographical note

Publisher Copyright:
© 2023 Wiley-VCH GmbH.

NREL Publication Number

  • NREL/JA-5700-85299

Keywords

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

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