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Elucidating the Energy Storage Mechanism of ZnMn2O4 as Promising Anode for Li-Ion Batteries

Abstract

Tetragonal spinel ZnMn2O4 provides an extremely high capacity as anode for Li-ion batteries owing to a conversion-type mechanism. In this work, nanoparticle-composed layered ZnMn2O4 is synthesized using a co-precipitation method. Calcination parameters are optimized through thermal gravimetric analysis and in situ high temperature synchrotron X-ray powder diffraction. The ZnMn2O4 shows an initial lithiation capacity of ~1400 mAh g-1 and a high reversible capacity of ~900 mAh g-1 at the specific current of 0.5 A g-1. In situ synchrotron X-ray powder diffraction reveals the phase evolution during the 1st cycle. The intermediate phase, tetragonal spinel LiZnMn2O4, forms and coexists with the original ZnMn2O4 during the 1st lithiation. Electrochemical impedance spectroscopy applied on varying potentials during the 1st cycle evidences the high Li+ diffusion coefficient and low electronic resistance of the electrode at the lithiated state, which enables high rate performance with 810 mAh g-1 at 1 A g-1 and 580 mAh g-1 at 2 A g-1. X-ray photoelectron spectroscopy reveals that the solid-electrolyte interphase is composed of LiOH and Li2CO3, which can contribute to the additional capacity. In addition, the Mn(II)/Mn(III) redox reaction appearing during 60th ~100th cycles is reported for the first time and can be another reason for the capacity increase upon cycling (the maximum capacity is ~1250 mAh g-1 at the 90th cycle). This redox reaction is facilitated by the increase of the electronic conductivity upon cycling. Based on these investigations, fundamental insights of the energy storage mechanism of ZnMn2O4 conversion anodes in Li-ion batteries are clarified. This work can shed light on the understanding of other conversion-type electrode materials.

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Publication details

The article was received on 01 Jul 2018, accepted on 03 Aug 2018 and first published on 07 Aug 2018


Article type: Paper
DOI: 10.1039/C8TA06294C
Citation: J. Mater. Chem. A, 2018, Accepted Manuscript
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    Elucidating the Energy Storage Mechanism of ZnMn2O4 as Promising Anode for Li-Ion Batteries

    Z. Zhao, G. Tian, A. Sarapulova, V. Trouillet, Q. Fu, U. Geckle, H. Ehrenberg and S. Dsoke, J. Mater. Chem. A, 2018, Accepted Manuscript , DOI: 10.1039/C8TA06294C

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