First-principles study on thermodynamic stability of the hybrid interfacial structure of LiMn2O4 cathode and carbonate electrolyte in Li-ion batteries

Daehyeon Choi, Joonhee Kang, Jinwoo Park, Byungchan Han

Research output: Contribution to journalArticle

3 Citations (Scopus)

Abstract

The solid electrolyte interphase (SEI) of Li-ion batteries (LIBs) has been extensively studied, with most research focused on the anode, because of its significant impact on the prolonged cycle life, initial capacity loss, and safety issues. Using first-principles density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations with the Hubbard correction, we examine the thermodynamic structure prediction and electrochemical stability of a spinel LiMn2O4 cathode interfaced with a carbonate electrolyte. The electronic energy levels of frontier orbitals of the electrolyte and the work function of the cathode offer clear characterization of the interfacial reactions. Our results based on both DFT calculations and AIMD simulations propose that the proton transfer mechanism at the hybrid interface is essential for initiating the SEI layer formation on the LiMn2O4 surface. Our results can be useful for identifying design concepts in the development of stable and high capacity LIBs with optimized electrodes and high-performance electrolytes.

Original languageEnglish
Pages (from-to)11592-11597
Number of pages6
JournalPhysical Chemistry Chemical Physics
Volume20
Issue number17
DOIs
Publication statusPublished - 2018 Jan 1

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Carbonates
Electrolytes
electric batteries
carbonates
Cathodes
Thermodynamic stability
cathodes
Solid electrolytes
solid electrolytes
electrolytes
thermodynamics
Density functional theory
Molecular dynamics
molecular dynamics
density functional theory
ions
Proton transfer
Computer simulation
Surface chemistry
Electron energy levels

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

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abstract = "The solid electrolyte interphase (SEI) of Li-ion batteries (LIBs) has been extensively studied, with most research focused on the anode, because of its significant impact on the prolonged cycle life, initial capacity loss, and safety issues. Using first-principles density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations with the Hubbard correction, we examine the thermodynamic structure prediction and electrochemical stability of a spinel LiMn2O4 cathode interfaced with a carbonate electrolyte. The electronic energy levels of frontier orbitals of the electrolyte and the work function of the cathode offer clear characterization of the interfacial reactions. Our results based on both DFT calculations and AIMD simulations propose that the proton transfer mechanism at the hybrid interface is essential for initiating the SEI layer formation on the LiMn2O4 surface. Our results can be useful for identifying design concepts in the development of stable and high capacity LIBs with optimized electrodes and high-performance electrolytes.",
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First-principles study on thermodynamic stability of the hybrid interfacial structure of LiMn2O4 cathode and carbonate electrolyte in Li-ion batteries. / Choi, Daehyeon; Kang, Joonhee; Park, Jinwoo; Han, Byungchan.

In: Physical Chemistry Chemical Physics, Vol. 20, No. 17, 01.01.2018, p. 11592-11597.

Research output: Contribution to journalArticle

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T1 - First-principles study on thermodynamic stability of the hybrid interfacial structure of LiMn2O4 cathode and carbonate electrolyte in Li-ion batteries

AU - Choi, Daehyeon

AU - Kang, Joonhee

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AU - Han, Byungchan

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AB - The solid electrolyte interphase (SEI) of Li-ion batteries (LIBs) has been extensively studied, with most research focused on the anode, because of its significant impact on the prolonged cycle life, initial capacity loss, and safety issues. Using first-principles density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations with the Hubbard correction, we examine the thermodynamic structure prediction and electrochemical stability of a spinel LiMn2O4 cathode interfaced with a carbonate electrolyte. The electronic energy levels of frontier orbitals of the electrolyte and the work function of the cathode offer clear characterization of the interfacial reactions. Our results based on both DFT calculations and AIMD simulations propose that the proton transfer mechanism at the hybrid interface is essential for initiating the SEI layer formation on the LiMn2O4 surface. Our results can be useful for identifying design concepts in the development of stable and high capacity LIBs with optimized electrodes and high-performance electrolytes.

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