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

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

doi:10.1021/acs.chemmater.0c01988

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

Journal Article · Tue Jul 14 00:00:00 EDT 2020 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.0c01988· OSTI ID:1756770

^[1]; ^[1]; ^[1]; Parajuli, Prakash ^[1]; Kumar, Khagesh ^[2]; Kim, Sanghyeon ^[1]; Yang, Mengxi ^[1]; Murphy, Megan ^[2]; ^[1]; ^[1]; ^[1]; ^[2]; ^[2]; ^[1]; Lapidus, Saul H. ^[1]; ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR)
Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR); Univ. of Illinois, Chicago, IL (United States)

We discuss how 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 O^2- exists. Mg/Mn antisite inversion in the spinel is lowered to similar to 10% via postannealing at 350 degrees 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 similar to 3.0 V (vs Mg/Mel. Clear remagnesiation upon first discharge, harvesting up to similar to 180 Wh/kg at 60 degrees 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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1756770

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 15 Vol. 32; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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