Revisiting Lithium- and Sodium-Ion Storage in Hard Carbon Anodes

Hoseong Kim, Jong Chan Hyun, Do Hoon Kim, Jin Hwan Kwak, Jin Bae Lee, Joon Ha Moon, Jaewon Choi, Hee Dae Lim, Seung Jae Yang, Hyeong Min Jin, Dong June Ahn, Kisuk Kang, Hyoung Joon Jin, Hyung Kyu Lim, Young Soo Yun

Research output: Contribution to journalArticlepeer-review

21 Citations (Scopus)

Abstract

The galvanostatic lithiation/sodiation voltage profiles of hard carbon anodes are simple, with a sloping drop followed by a plateau. However, a precise understanding of the corresponding redox sites and storage mechanisms is still elusive, which hinders further development in commercial applications. Here, a comprehensive comparison of the lithium- and sodium-ion storage behaviors of hard carbon is conducted, yielding the following key findings: 1) the sloping voltage section is presented by the lithium-ion intercalation in the graphitic lattices of hard carbons, whereas it mainly arises from the chemisorption of sodium ions on their inner surfaces constituting closed pores, even if the graphitic lattices are unoccupied; 2) the redox sites for the plateau capacities are the same as those for the closed pores regardless of the alkali ions; 3) the sodiation plateau capacities are mostly determined by the volume of the available closed pore, whereas the lithiation plateau capacities are primarily affected by the intercalation propensity; and 4) the intercalation preference and the plateau capacity have an inverse correlation. These findings from extensive characterizations and theoretical investigations provide a relatively clear elucidation of the electrochemical footprint of hard carbon anodes in relation to the redox mechanisms and storage sites for lithium and sodium ions, thereby providing a more rational design strategy for constructing better hard carbon anodes.

Original languageEnglish
Article number2209128
JournalAdvanced Materials
Volume35
Issue number12
DOIs
Publication statusPublished - 2023 Mar 23

Bibliographical note

Funding Information:
H.K. and J.C.H. contributed equally to this work. This research was supported by the Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (Grant Nos. NRF‐ 2019R1A2C1084836 and NRF‐2021R1A4A2001403) and the Ministry of Science and ICT (Grant No. NRF‐2022R1C1C1011484). This work was supported by the KU‐KIST School Program.

Funding Information:
H.K. and J.C.H. contributed equally to this work. This research was supported by the Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (Grant Nos. NRF- 2019R1A2C1084836 and NRF-2021R1A4A2001403) and the Ministry of Science and ICT (Grant No. NRF-2022R1C1C1011484). This work was supported by the KU-KIST School Program.

Publisher Copyright:
© 2023 Wiley-VCH GmbH.

Keywords

  • alkali-ion storage mechanism
  • hard carbon anode
  • intercalation propensity
  • lithium-ion batteries
  • pore-filling mechanism
  • sodium-ion batteries

ASJC Scopus subject areas

  • General Materials Science
  • Mechanics of Materials
  • Mechanical Engineering

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