Ionic Conduction Mechanism and Design of Metal-Organic Framework Based Quasi-Solid-State Electrolytes

被引：75

作者：

Hou, Tingzheng ^{[1
,2
]}

Xu, Wentao ^{[3
]}

Pei, Xiaokun ^{[3
]}

Jiang, Lu ^{[1
,5
]}

Yaghi, Omar M. ^{[3
]}

Persson, Kristin A. ^{[1
,4
]}

机构：

[1] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA

[2] Lawrence Berkeley Natl Lab, Energy Technol Area, Berkeley, CA 94720 USA

[3] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA

[4] Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA

[5] Lawrence Berkeley Natl Lab, Mat Sci Div, Berkeley, CA 94720 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2022年 / 144卷 / 30期

关键词：

TEMPERATURE; MORPHOLOGY; TRANSPORT; LIPF6;

D O I：

10.1021/jacs.2c03710

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

We report the theoretical and experimental investigation of two polyoxometalate-based metal-organic frameworks (MOFs), [(MnMo6)(2)(TFPM)](imine) and [(AlMo6)(2)(TFPM)](imine), as quasi-solid-state electrolytes. Classical molecular dynamics coupled with quantum chemistry and grand canonical Monte Carlo are utilized to model the corresponding diffusion and ionic conduction in the two materials. Using different approximate levels of ion diffusion behavior, the primary ionic conduction mechanism was identified as solvent-assisted hopping (> 77%). Detailed static and dynamic solvation structures were obtained to interpret Li+ motion with high spatial and temporal resolution. A rationally designed noninterpenetrating MOF-688(one-fold) material is proposed to achieve 6-8 times better performance (1.6-1.7 mS cm(-1)) than the current state-of-the-art (0.19-0.35 mS cm(-1)).

引用

页码：13446 / 13450

页数：5

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