Mixed Ionic–Electronic Conductor of Perovskite LixLayMO3−δ toward Carbon-Free Cathode for Reversible Lithium–Air Batteries

Sang Bok Ma, Hyuk Jae Kwon, Mokwon Kim, Seong Min Bak, Hyunpyo Lee, Steven N. Ehrlich, Jeong Ju Cho, Dongmin Im, Dong Hwa Seo

Research output: Contribution to journalArticlepeer-review


Mixed ionic–electronic conductors (MIECs) can play a pivotal role in achieving high energies and power densities in rechargeable batteries owing to their ability to simultaneously conduct ions and electrons. Herein, a new strategy is proposed wherein late 3d transition metals (TMs) are substituted into a perovskite Li-ion conductor to transform it into a Li-containing MIEC. First-principles calculations show that perovskite LixLayMO3 with late 3d TMs have a low oxygen vacancy formation energy, implying high electron carrier concentrations corresponding to high electronic conductivity. The activation barriers for Li diffusion in LixLayMO3 (M = Ti, Cr, Mn, Fe, and Co) are below 0.411 eV, resulting in high Li-ion conductivity. The designed perovskites of Li0.34La0.55MnO3−δ experimentally prove to have high electronic (2.04 × 10−3 S cm−1) and Li-ion (8.53 × 10−5 S cm−1) conductivities, and when applied in a carbon-free cathode of a Li–air cell, they deliver superior reversibility at 0.21 mAh cm−2 over 100 charge/discharge cycles while avoiding the degradation associated with carbonaceous materials. This strategy enables the effective design of Li-conducting MIEC and reversible Li–air batteries.

Original languageEnglish
Article number2001767
JournalAdvanced Energy Materials
Issue number38
Publication statusPublished - 2020 Oct 1

Bibliographical note

Funding Information:
S.‐M.B. at Brookhaven National Laboratory was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) Program under contract DE‐SC0012704. The XAS research was performed at beamline 7‐BM (QAS) of the National Synchrotron Light Source II, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE‐SC0012704. D.‐H.S. was supported by the 2020 Research Fund (1.200092.01) of Ulsan National Institute of Science & Technology. The computational work was supported by the Supercomputing Center/Korea Institute of Science and Technology Information with supercomputing resources including technical support (KSC‐2018‐CRE‐0006 to D.‐H.S.).

Publisher Copyright:
© 2020 Wiley-VCH GmbH

All Science Journal Classification (ASJC) codes

  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)


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