Supramolecular metal-organic frameworks that display high homogeneous and heterogeneous photocatalytic activity for H2 production

Jia Tian, Zi-Yue Xu, Dan-Wei Zhang, Hui Wang (), Song-Hai Xie, Da-Wen Xu, Yuan-Hang Ren, Hao Wang, Yi Liu () and Zhan-Ting Li ()
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Jia Tian: Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Fudan University
Zi-Yue Xu: Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Fudan University
Dan-Wei Zhang: Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Fudan University
Hui Wang: Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Fudan University
Song-Hai Xie: Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Fudan University
Da-Wen Xu: Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Fudan University
Yuan-Hang Ren: Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Fudan University
Hao Wang: Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Fudan University
Yi Liu: The Molecular Foundry, Lawrence Berkeley National Laboratory
Zhan-Ting Li: Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Fudan University

Nature Communications, 2016, vol. 7, issue 1, 1-9

Abstract: Abstract Self-assembly has a unique presence when it comes to creating complicated, ordered supramolecular architectures from simple components under mild conditions. Here, we describe a self-assembly strategy for the generation of the first homogeneous supramolecular metal-organic framework (SMOF-1) in water at room temperature from a hexaarmed [Ru(bpy)3]2+-based precursor and cucurbit[8]uril (CB[8]). The solution-phase periodicity of this cubic transition metal-cored supramolecular organic framework (MSOF) is confirmed by small-angle X-ray scattering and diffraction experiments, which, as supported by TEM imaging, is commensurate with the periodicity in the solid state. We further demonstrate that SMOF-1 adsorbs anionic Wells−Dawson-type polyoxometalates (WD-POMs) in a one-cage-one-guest manner to give WD-POM@SMOF-1 hybrid assemblies. Upon visible-light (500 nm) irradiation, such hybrids enable fast multi-electron injection from photosensitive [Ru(bpy)3]2+ units to redox-active WD-POM units, leading to efficient hydrogen production in aqueous media and in organic media. The demonstrated strategy opens the door for the development of new classes of liquid-phase and solid-phase ordered porous materials.

Date: 2016
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DOI: 10.1038/ncomms11580

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