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A Metal–Organic Framework of Organic Vertices and Polyoxometalate Linkers as a Solid-State Electrolyte

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journal contribution
posted on 25.10.2019, 14:47 by Wentao Xu, Xiaokun Pei, Christian S. Diercks, Hao Lyu, Zhe Ji, Omar M. Yaghi
A new three-dimensional metal–organic framework (MOF) was synthesized by linking ditopic amino functionalized polyoxometalate [N­(C4H9)4]3[MnMo6O18­{(OCH2)3CNH2}2] with 4-connected tetrahedral tetrakis­(4-formyl­phenyl)­methane building units through imine condensation. The structure of this MOF, termed MOF-688, was solved by single crystal X-ray diffraction and found to be triply interpenetrated diamond-based dia topology. Tetrabutylammonium cations fill the pores and balance the charge of the anionic framework. They can be exchanged with lithium ions to give high ionic conductivity (3.4 × 10–4 S cm–1 at 20 °C), a high lithium ion transference number (tLi+ = 0.87), and low interfacial resistance (353 Ω) against metallic lithiumproperties that make it ideally suited as a solid-state electrolyte. Indeed, a prototype lithium metal battery constructed using MOF-688 as the solid electrolyte can be cycled at room temperature with a practical current density of ∼0.2 C.