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Reversible Li+Storage in a LiMnTiO4Spinel and Its Structural Transition Mechanisms

Chen, Ruiyong and Knapp, Michael and Yavuz, Murat and Heinzmann, Ralf and Wang, Di and Ren, Shuhua and Trouillet, Vanessa and Lebedkin, Sergei and Doyle, Stephen and Hahn, Horst and Ehrenberg, Helmut and Indris, Sylvio (2014):
Reversible Li+Storage in a LiMnTiO4Spinel and Its Structural Transition Mechanisms.
118, In: The Journal of Physical Chemistry C, (24), ACS Publishing, pp. 12608-12616, ISSN 1932-7447, [Online-Edition: http://dx.doi.org/10.1021/jp501618n],
[Article]

Abstract

In this work, LiMnTiO4 (a structural analogue of classic spinel LiMn2O4) with a disordered cubic spinel structure (Fd (3) over barm) has been synthesized by a low-temperature sol-gel route. The as-obtained LiMnTiO4 exhibits excellent cycling stability in a wide voltage range from 1.5 to 4.8 V with high discharge capacities of 290, 250, and 140 mA h g(-1) at a C/40, C/19, and 1C rate, respectively. Combined long- and short-range structural characterization techniques are used to reveal the correlation between structure and electrochemical behavior. During cycling, the charge/discharge profiles of LiMnTiO4 evolve from initially two well-separated plateaus into sloping regimes. In the early stage of discharge, LiMnTiO4 undergoes phase transitions from an initial spinel phase to mixtures of predominant rock-salt (Fm (3) over barm) and tetragonal (I4(1)/amd) structures along with a decrease in crystallite size from 12 nm to 3 to 4 nm. During further cycling, the spinel/rock-salt phase transition was found to be reversible with the cubic framework remaining intact. The presence of the tetragonal phase after the first discharge suggests that the Mn3+ Jahn-Teller distortion is partially involved during lithiation from Li1-yMn3+yTiO4 to Li1+xMn3-xTiO4 and the fraction of such a tetragonal phase remains at about 30-40% during subsequent cycling.

Item Type: Article
Erschienen: 2014
Creators: Chen, Ruiyong and Knapp, Michael and Yavuz, Murat and Heinzmann, Ralf and Wang, Di and Ren, Shuhua and Trouillet, Vanessa and Lebedkin, Sergei and Doyle, Stephen and Hahn, Horst and Ehrenberg, Helmut and Indris, Sylvio
Title: Reversible Li+Storage in a LiMnTiO4Spinel and Its Structural Transition Mechanisms
Language: English
Abstract:

In this work, LiMnTiO4 (a structural analogue of classic spinel LiMn2O4) with a disordered cubic spinel structure (Fd (3) over barm) has been synthesized by a low-temperature sol-gel route. The as-obtained LiMnTiO4 exhibits excellent cycling stability in a wide voltage range from 1.5 to 4.8 V with high discharge capacities of 290, 250, and 140 mA h g(-1) at a C/40, C/19, and 1C rate, respectively. Combined long- and short-range structural characterization techniques are used to reveal the correlation between structure and electrochemical behavior. During cycling, the charge/discharge profiles of LiMnTiO4 evolve from initially two well-separated plateaus into sloping regimes. In the early stage of discharge, LiMnTiO4 undergoes phase transitions from an initial spinel phase to mixtures of predominant rock-salt (Fm (3) over barm) and tetragonal (I4(1)/amd) structures along with a decrease in crystallite size from 12 nm to 3 to 4 nm. During further cycling, the spinel/rock-salt phase transition was found to be reversible with the cubic framework remaining intact. The presence of the tetragonal phase after the first discharge suggests that the Mn3+ Jahn-Teller distortion is partially involved during lithiation from Li1-yMn3+yTiO4 to Li1+xMn3-xTiO4 and the fraction of such a tetragonal phase remains at about 30-40% during subsequent cycling.

Journal or Publication Title: The Journal of Physical Chemistry C
Volume: 118
Number: 24
Publisher: ACS Publishing
Divisions: 11 Department of Materials and Earth Sciences > Material Science > Joint Research Laboratory Nanomaterials
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences
Date Deposited: 10 Feb 2016 09:55
Official URL: http://dx.doi.org/10.1021/jp501618n
Identification Number: doi:10.1021/jp501618n
Funders: This work was financially supported by the German Federal Ministry of Education and Research and the "Helmholtz Initiative for Mobile/Stationary Energy Storage Systems".
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