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

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...

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Veröffentlicht in:Chemistry of materials 2020-08, Vol.32 (15), p.6577-6587
Hauptverfasser: Kwon, Bob Jin, Yin, Liang, Park, Haesun, Parajuli, Prakash, Kumar, Khagesh, Kim, Sanghyeon, Yang, Mengxi, Murphy, Megan, Zapol, Peter, Liao, Chen, Fister, Timothy T, Klie, Robert F, Cabana, Jordi, Vaughey, John T, Lapidus, Saul H, Key, Baris
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container_end_page 6587
container_issue 15
container_start_page 6577
container_title Chemistry of materials
container_volume 32
creator Kwon, Bob Jin
Yin, Liang
Park, Haesun
Parajuli, Prakash
Kumar, Khagesh
Kim, Sanghyeon
Yang, Mengxi
Murphy, Megan
Zapol, Peter
Liao, Chen
Fister, Timothy T
Klie, Robert F
Cabana, Jordi
Vaughey, John T
Lapidus, Saul H
Key, Baris
description 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.
doi_str_mv 10.1021/acs.chemmater.0c01988
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subjects Electrodes
ENERGY STORAGE
Lattices
Oxides
Spinel
Transition metals
title High Voltage Mg-Ion Battery Cathode via a Solid Solution Cr–Mn Spinel Oxide
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