Demonstration of Magnesium Intercalation into a High-Voltage Oxide Electrode

(Top) Enlarged view of atomic-resolution scanning transmission electron microscopy image from spinel-type Mn2O4 [100] reduced in an aqueous Mg2+ electrolyte. Characteristic “diamond” unit cell is overlaid, indicating the atomic positions of Mn, O, and Mg; clear occupancy of the tetrahedral sites is shown.
(Bottom) Results of an X-ray spectroscopy (EDX) line scan, acquired horizontally through the center of two “diamond” unit cells. This confirms the presence of Mg in the tetrahedral sites, and the expected atomic arrangement of Mn-O-Mg-Mg-O-Mn in the MgMn2O4 structure.

Scientific Achievement

First demonstration of reversible insertion of multivalent magnesium ions (Mg2+) into a spinel-type manganese oxide (Mn2O4), using multi-modal characterization

Significance and Impact

  • Proof of Mg2+ insertion provides an avenue to designing a high voltage cathode for a magnesium-based battery that surpasses current lithium-ion technology
  • Breakthrough enabled by JCESR Sprint establishing strategic collaborations on specific fundamental issues

Research Details

  • Reversible Mg intercalation into Mn2O4 observed in both aqueous and non-aqueous electrolytes. Results from four different tools provided insight at different scales.
  • Reaction between Mn2O4 and MgMn2O4 observed at an average voltage of 2.9 V vs. Mg2+/Mg0. Theoretical specific energy: 783 Wh/kg (compared to 400 Wh/kg in today’s lithium-ion).

Work performed at the University of Illinois at Chicago and SLAC National Accelerator Laboratory (JCESR partners) and Argonne National Laboratory (JCESR managing partner) by C Kim, PJ Phillips, B Key, T Yi, D Nordlund, Y-S Yu, RD Bayliss, S-D Han, M He, AK Burrell, RF Klie and J Cabana, Advanced Materials

DOI: 10.1002/adma.201500083

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