Fe3+-Derived Boosted Charge Transfer in an FeSi4P4Anode for Ultradurable Li-Ion Batteries

Mahboobeh Nazarian-Samani, Masoud Nazarian-Samani, Safa Haghighat-Shishavan, Kwang Bum Kim

Research output: Contribution to journalArticlepeer-review

4 Citations (Scopus)

Abstract

Ion and electron transportation determine the electrochemical performance of anodes in metal-ion batteries. This study demonstrates the advantage of charge transfer over mass transport in ensuring ultrastable electrochemical performance. Additionally, charge transfer governs the quality, composition, and morphology of a solid-electrolyte interphase (SEI) film. We develop FeSi4P4-carbon nanotube (FSPC) and reduced-FeSi4P4-carbon nanotube (R-FSPC) heterostructures. The FSPC contains abundant Fe3+cations and negligible pore contents, whereas R-FSPC predominantly comprises Fe2+and an abundance of nanopores and vacancies. The copious amount of Fe3+ions in FSPC significantly improves charge transfer during Li-ion battery tests and leads to the formation of a thin monotonic SEI film. This prevents the formation of detrimental LiP and crystalline-Li3.75Si phases and the aggregation of discharging/recharging products and guarantees the reformation of FeSi4P4nanocrystals during delithiation. Thus, FSPC delivers a high initial Coulombic efficiency (>90%), exceptional rate capability (616 mAh g-1at 15 A g-1), and ultrastable symmetric/asymmetric cycling performance (>1000 cycles at ultrahigh current densities). This study deepens our understanding of the effects of electron transport on regulating the structural and electrochemical properties of electrode materials in high-performance batteries.

Original languageEnglish
Pages (from-to)12606-12619
Number of pages14
JournalACS Nano
Volume16
Issue number8
DOIs
Publication statusPublished - 2022 Aug 23

Bibliographical note

Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.

All Science Journal Classification (ASJC) codes

  • General Materials Science
  • General Engineering
  • General Physics and Astronomy

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