Controlled Nitrogen Doping in Crumpled Graphene for Improved Alkali Metal-Ion Storage under Low-Temperature Conditions

Kyungbin Lee, Michael J. Lee, Jeonghoon Lim, Kun Ryu, Mochen Li, Suguru Noda, Seok Joon Kwon*, Seung Woo Lee*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

The significant performance decay in conventional graphite anodes under low-temperature conditions is attributed to the slow diffusion of alkali metal ions, requiring new strategies to enhance the charge storage kinetics at low temperatures. Here, nitrogen (N)-doped defective crumpled graphene (NCG) is employed as a promising anode to enable stable low-temperature operation of alkali metal-ion storage by exploiting the surface-controlled charge storage mechanisms. At a low temperature of −40 °C, the NCG anodes maintain high capacities of ≈172 mAh g−1 for lithium (Li)-ion, ≈107 mAh g−1 for sodium (Na)-ion, and ≈118 mAh g−1 for potassium (K)-ion at 0.01 A g−1 with outstanding rate-capability and cycling stability. A combination of density functional theory (DFT) and electrochemical analysis further reveals the role of the N-functional groups and defect sites in improving the utilization of the surface-controlled charge storage mechanisms. In addition, the full cell with the NCG anode and a LiFePO4 cathode shows a high capacity of ≈73 mAh g−1 at 0.5 °C even at −40 °C. The results highlight the importance of utilizing the surface-controlled charge storage mechanisms with controlled defect structures and functional groups on the carbon surface to improve the charge storage performance of alkali metal-ion under low-temperature conditions.

Original languageEnglish
Article number2209775
JournalAdvanced Functional Materials
Volume33
Issue number2
DOIs
Publication statusPublished - 2023 Jan 10

Keywords

  • crumpled graphene
  • lithium-ion batteries
  • low-temperature operation
  • nitrogen-doping
  • surface-controlled charge storages

ASJC Scopus subject areas

  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics

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