A stable metal-covalent-supramolecular organic framework hybrid: enrichment of catalysts for visible light-induced hydrogen production

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Abstract

Cubic metal-covalent-supramolecular organic framework (MCSOF-1) hybrid has been created from the reaction of two molecular components and subsequent co-assembly with cucurbit[8]uril (CB[8]) in water. In the presence of CB[8], [Ru(bpy)3]2+ -based acylhydrazine 1·2Cl reacted with aldehyde 2·Cl to quantitatively yield six-armed precursor 3·8Cl through the generation of MCSOF-1. MCSOF-1 combines the structural features of metal-, covalent- and supramolecular organic frameworks. Its periodicity in water and in the solid state was confirmed by synchrotron X-ray scattering and diffraction experiments. MCSOF-1 could enrich discrete anionic polyoxometalates (POMs), maintain periodicity in acidic medium, and remarkably facilitate visible light-induced electron transfer from its [Ru(bpy)3]2+ units to enriched POMs, leading to enhanced catalysis of the POMs for the reduction of proton to H2 in both aqueous (homogeneous) and organic (heterogeneous) media.

Keywords

supramolecular organic framework self-assembly cucurbitu[8]ril photocatalysis hydrogen production 
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Notes

Acknowledgments

This work was supported by the National Natural Science Foundation of China (21529201, 21432004, 91527301), the Molecular Foundry, Lawrence Berkeley National Laboratory, and the Office of Science, Office of Basic Energy Sciences, Scientific User Facilities Division, of the U.S. Department of Energy (DE-AC02- 05CH11231). We thank the Shanghai Synchrotron Radiation Facility for providing BL16B1 and BL14B1 beamlines for collecting the synchrotron X-ray scattering and diffraction data, and the SIBYLS Beamline 12.3.1 of the Advanced Light Source, Lawrence Berkeley National Laboratory, for collecting solutionphase synchrotron small-angle X-ray scattering data.

Supplementary material

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Copyright information

© Science China Press and Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  1. 1.Department of Chemistry, Collaborative Innovation Centre of Chemistry for Energy Materials (iChEM), Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsFudan UniversityShanghaiChina
  2. 2.The Molecular FoundryLawrence Berkeley National LaboratoryBerkeleyUSA

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