Comparative computational investigation of N and F substituted polyoxoanionic compounds The case of Li2FeSiO4 electrode material

被引：33

作者：

Armand, M. ^{[2
]}

Tarascon, J. -M. ^{[2
]}

Arroyo-de Dompablo, M. E. ^{[1
]}

机构：

[1] Univ Complutense Madrid, Fac Quim, E-28040 Madrid, Spain

[2] Univ Picardie Jules Verne, LRCS, UMR CNRS 6007, F-80039 Amiens, France

来源：

ELECTROCHEMISTRY COMMUNICATIONS | 2011年 / 13卷 / 10期

关键词：

Li2FeSiO4; Electrode materials; DFT; Silicates;

D O I：

10.1016/j.elecom.2011.06.027

中图分类号：

O646 [电化学、电解、磁化学];

学科分类号：

081704 ;

摘要：

First principles calculations are used to anticipate the electrochemistry of polyoxoanionic materials consisting of XO(4-y)A(y) (A = F, N) groups. As an illustrative case, this work focuses on the effect of either N or F for O substitution upon the electrochemical properties of Li2FeSiO4. Within the Pmn2(1)-Li2FeSiO4 structure, virtual models of Li2Fe22.5+SiO3.5N0.5 and Li1.5Fe2+SiO3.5F0.5 have been analyzed. We predict that the lithium deinsertion voltage associated to the Fe3+/Fe4+ redox couple is decreased by both substituents. The high theoretical specific capacity of Li2FeSiO4 (330 mAh/g) could be retained in N-substituted silicates thanks to the oxidation of N3- anions, whilst Li1.5Fe2+SiO3.5F0.5 has a lower specific capacity inherent to the F substitution. Substitution of N/F for O will respectively improve/worsen the electrode characteristics of Li2FeSiO4. (C) 2011 Elsevier B.V. All rights reserved.

引用

页码：1047 / 1050

页数：4

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