High Voltage Mg-Ion Battery Cathode via a Solid Solution Cr-Mn Spinel Oxide

Bob Jin Kwon; Liang Yin; Haesun Park; Prakash Parajuli; Khagesh Kumar; Sanghyeon Kim; Mengxi Yang; Megan Murphy; Peter Zapol; Chen Liao; Timothy T. Fister; Robert F. Klie; Jordi Cabana; John T. Vaughey; Saul H. Lapidus; Baris Key

doi:10.1021/acs.chemmater.0c01988

High Voltage Mg-Ion Battery Cathode via a Solid Solution Cr-Mn Spinel Oxide

Bob Jin Kwon
, Liang Yin
, Haesun Park
, Prakash Parajuli
, Khagesh Kumar
, Sanghyeon Kim
, Mengxi Yang
, Megan Murphy
, Peter Zapol
, Chen Liao
, Timothy T. Fister
, Robert F. Klie
, Jordi Cabana
, John T. Vaughey
, Saul H. Lapidus
, Baris Key

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69 Scopus citations

Abstract

Lattice Mg2+ in a tailored solid solution spinel, MgCrMnO4, is electrochemically utilized at high Mn-redox potentials in a nonaqueous electrolyte. Complementary evidence from experimental and theoretical analyses supports bulk Mg2+ (de)intercalation throughout the designed oxide frame where strong electrostatic interaction between Mg2+ and O2- exists. Mg/Mn antisite inversion in the spinel is lowered to ∼10% via postannealing at 350 °C to further improve Mg2+ mobility. Spinel lattice is preserved upon removal of Mg2+ without any phase transformations, denoting structural stability at the charged state at a high potential ∼3.0 V (vs Mg/Mg2+). Clear remagnesiation upon first discharge, harvesting up to ∼180 Wh/kg at 60 °C is shown. In the remagnesiated state, insertion of Mg2+ into interstitial sites in the spinel is detected, possibly resulting in partial reversibility which needs to be addressed for structural stability. The observations constitute a first clear path to the development of a practical high voltage Mg-ion cathode using a spinel oxide.

Original language	English
Pages (from-to)	6577-6587
Number of pages	11
Journal	Chemistry of Materials
Volume	32
Issue number	15
DOIs	https://doi.org/10.1021/acs.chemmater.0c01988
State	Published - Aug 11 2020

Funding

This work is solely supported by the Joint Center for Energy Storage Research (JCESR) and Energy Innovation Hub funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences. The acquisition of the UIC JEOL JEM ARM200CF was supported by an MRI-R grant from the National Science Foundation (Grant No. DMR-0959470) and the upgraded Gatan Continuum spectrometer was supported by a grant from the NSF (DMR-1626065). This work made use of instruments in the Electron Microscopy Service at the Research Resources Center at UIC. Department of Energy (DOE) Office of Science user facility operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357. Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. 2

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10.1021/acs.chemmater.0c01988

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@article{ef5f276dd1484b0fbca5add6e7d7652c,

title = "High Voltage Mg-Ion Battery Cathode via a Solid Solution Cr-Mn Spinel Oxide",

abstract = "Lattice Mg2+ in a tailored solid solution spinel, MgCrMnO4, is electrochemically utilized at high Mn-redox potentials in a nonaqueous electrolyte. Complementary evidence from experimental and theoretical analyses supports bulk Mg2+ (de)intercalation throughout the designed oxide frame where strong electrostatic interaction between Mg2+ and O2- exists. Mg/Mn antisite inversion in the spinel is lowered to ∼10\% via postannealing at 350 °C to further improve Mg2+ mobility. Spinel lattice is preserved upon removal of Mg2+ without any phase transformations, denoting structural stability at the charged state at a high potential ∼3.0 V (vs Mg/Mg2+). Clear remagnesiation upon first discharge, harvesting up to ∼180 Wh/kg at 60 °C is shown. In the remagnesiated state, insertion of Mg2+ into interstitial sites in the spinel is detected, possibly resulting in partial reversibility which needs to be addressed for structural stability. The observations constitute a first clear path to the development of a practical high voltage Mg-ion cathode using a spinel oxide.",

author = "Kwon, \{Bob Jin\} and Liang Yin and Haesun Park and Prakash Parajuli and Khagesh Kumar and Sanghyeon Kim and Mengxi Yang and Megan Murphy and Peter Zapol and Chen Liao and Fister, \{Timothy T.\} and Klie, \{Robert F.\} and Jordi Cabana and Vaughey, \{John T.\} and Lapidus, \{Saul H.\} and Baris Key",

note = "Publisher Copyright: Copyright {\textcopyright} 2020 American Chemical Society.",

year = "2020",

month = aug,

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doi = "10.1021/acs.chemmater.0c01988",

language = "English",

volume = "32",

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T1 - High Voltage Mg-Ion Battery Cathode via a Solid Solution Cr-Mn Spinel Oxide

AU - Kwon, Bob Jin

AU - Yin, Liang

AU - Park, Haesun

AU - Parajuli, Prakash

AU - Kumar, Khagesh

AU - Kim, Sanghyeon

AU - Yang, Mengxi

AU - Murphy, Megan

AU - Zapol, Peter

AU - Liao, Chen

AU - Fister, Timothy T.

AU - Klie, Robert F.

AU - Cabana, Jordi

AU - Vaughey, John T.

AU - Lapidus, Saul H.

AU - Key, Baris

PY - 2020/8/11

Y1 - 2020/8/11

N2 - Lattice Mg2+ in a tailored solid solution spinel, MgCrMnO4, is electrochemically utilized at high Mn-redox potentials in a nonaqueous electrolyte. Complementary evidence from experimental and theoretical analyses supports bulk Mg2+ (de)intercalation throughout the designed oxide frame where strong electrostatic interaction between Mg2+ and O2- exists. Mg/Mn antisite inversion in the spinel is lowered to ∼10% via postannealing at 350 °C to further improve Mg2+ mobility. Spinel lattice is preserved upon removal of Mg2+ without any phase transformations, denoting structural stability at the charged state at a high potential ∼3.0 V (vs Mg/Mg2+). Clear remagnesiation upon first discharge, harvesting up to ∼180 Wh/kg at 60 °C is shown. In the remagnesiated state, insertion of Mg2+ into interstitial sites in the spinel is detected, possibly resulting in partial reversibility which needs to be addressed for structural stability. The observations constitute a first clear path to the development of a practical high voltage Mg-ion cathode using a spinel oxide.

AB - Lattice Mg2+ in a tailored solid solution spinel, MgCrMnO4, is electrochemically utilized at high Mn-redox potentials in a nonaqueous electrolyte. Complementary evidence from experimental and theoretical analyses supports bulk Mg2+ (de)intercalation throughout the designed oxide frame where strong electrostatic interaction between Mg2+ and O2- exists. Mg/Mn antisite inversion in the spinel is lowered to ∼10% via postannealing at 350 °C to further improve Mg2+ mobility. Spinel lattice is preserved upon removal of Mg2+ without any phase transformations, denoting structural stability at the charged state at a high potential ∼3.0 V (vs Mg/Mg2+). Clear remagnesiation upon first discharge, harvesting up to ∼180 Wh/kg at 60 °C is shown. In the remagnesiated state, insertion of Mg2+ into interstitial sites in the spinel is detected, possibly resulting in partial reversibility which needs to be addressed for structural stability. The observations constitute a first clear path to the development of a practical high voltage Mg-ion cathode using a spinel oxide.

UR - https://www.scopus.com/pages/publications/85093364288

U2 - 10.1021/acs.chemmater.0c01988

DO - 10.1021/acs.chemmater.0c01988

M3 - Article

AN - SCOPUS:85093364288

SN - 0897-4756

VL - 32

SP - 6577

EP - 6587

JO - Chemistry of Materials

JF - Chemistry of Materials

IS - 15

ER -

High Voltage Mg-Ion Battery Cathode via a Solid Solution Cr-Mn Spinel Oxide

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