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

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13 Citations (Scopus)


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
Issue number17
Publication statusPublished - 2018

Bibliographical note

Funding Information:
This research was supported by the Global Frontier Program through the Global Frontier Hybrid Interface Materials (GFHIM) of National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (Project No. 2013M3A6B1078882).

Publisher Copyright:
© 2018 the Owner Societies.

All Science Journal Classification (ASJC) codes

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


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