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Title: Supramolecular metal-organic frameworks that display high homogeneous and heterogeneous photocatalytic activity for H 2 production

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.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [1]
  1. Fudan Univ., Shanghai (China). Dept. of Chemistry
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; metal-organic frameworks; photocatalysis
OSTI Identifier:
1379333

Tian, Jia, Xu, Zi-Yue, Zhang, Dan-Wei, Wang, Hui, Xie, Song-Hai, Xu, Da-Wen, Ren, Yuan-Hang, Wang, Hao, Liu, Yi, and Li, Zhan-Ting. Supramolecular metal-organic frameworks that display high homogeneous and heterogeneous photocatalytic activity for H2 production. United States: N. p., Web. doi:10.1038/ncomms11580.
Tian, Jia, Xu, Zi-Yue, Zhang, Dan-Wei, Wang, Hui, Xie, Song-Hai, Xu, Da-Wen, Ren, Yuan-Hang, Wang, Hao, Liu, Yi, & Li, Zhan-Ting. Supramolecular metal-organic frameworks that display high homogeneous and heterogeneous photocatalytic activity for H2 production. United States. doi:10.1038/ncomms11580.
Tian, Jia, Xu, Zi-Yue, Zhang, Dan-Wei, Wang, Hui, Xie, Song-Hai, Xu, Da-Wen, Ren, Yuan-Hang, Wang, Hao, Liu, Yi, and Li, Zhan-Ting. 2016. "Supramolecular metal-organic frameworks that display high homogeneous and heterogeneous photocatalytic activity for H2 production". United States. doi:10.1038/ncomms11580. https://www.osti.gov/servlets/purl/1379333.
@article{osti_1379333,
title = {Supramolecular metal-organic frameworks that display high homogeneous and heterogeneous photocatalytic activity for H2 production},
author = {Tian, Jia and Xu, Zi-Yue and Zhang, Dan-Wei and Wang, Hui and Xie, Song-Hai and Xu, Da-Wen and Ren, Yuan-Hang and Wang, Hao and Liu, Yi and Li, Zhan-Ting},
abstractNote = {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.},
doi = {10.1038/ncomms11580},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {5}
}