Journal
CHEMISTRY OF MATERIALS
Volume 32, Issue 2, Pages 663-670Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.9b02450
Keywords
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Funding
- Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub - US Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES)
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-ACO2-06CH11357]
- Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy
- DOE Office of Science, Office of Biological and Environmental Research at Pacific Northwest National Laboratory (PNNL)
- DOE Office of Science, Physical Science Laboratory at Pacific Northwest National Laboratory (PNNL)
- DOE [DE-ACOS76RL01830]
- Oxford Martin Programme for Integrating Renewable Energy at the Oxford Martin School, University of Oxford
- Ramsay Memorial Trust
- University College London
- EPSRC [EP/S003053/1] Funding Source: UKRI
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Mg batteries utilizing oxide cathodes can theoretically surpass the energy density of current Li-ion technologies. The absence of functional devices so far has been ascribed to impeded Mg2+ migration within oxides, which severely handicaps intercalation reactions at the cathode. Broadly, knowledge of divalent cation migration in solid frameworks is surprisingly deficient. Here, we present a combined experimental and theoretical study of Mg migration within three spinel oxides, which reveal critical features that influence it. Experimental activation energies for a Mg2+ hop to 500 an adjacent vacancy, as low as similar to 0.6 eV, are reported. These barriers are low enough to support functional electrodes based on the intercalation of Mg2+. Subsequent electrochemical experiments demonstrate that significant demagnesiation is indeed possible, but the challenges instead lie with the chemical stability of the oxidized states. Our findings enhance the understanding of cation transport in solid structures and renew the prospects of finding materials capable of high density of energy storage.
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