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

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

doi:10.1038/ncomms11580

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

Journal Article · Mon May 09 20:00:00 EDT 2016 · Nature Communications

DOI: https://doi.org/10.1038/ncomms11580 · OSTI ID:1379333

Tian, Jia ^[1]; Xu, Zi-Yue ^[1]; Zhang, Dan-Wei ^[1]; Wang, Hui ^[1]; Xie, Song-Hai ^[1]; Xu, Da-Wen ^[1]; Ren, Yuan-Hang ^[1]; Wang, Hao ^[1]; Liu, Yi ^[2]; Li, Zhan-Ting ^[1]

Fudan Univ., Shanghai (China). Dept. of Chemistry
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry

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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1379333

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 7; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Surveying macrocyclic chemistry: from flexible crown ethers to rigid cyclophanes Liu, Zhichang; Nalluri, Siva Krishna Mohan; Stoddart, J. Fraser Chemical Society Reviews, Vol. 46, Issue 9 https://doi.org/10.1039/c7cs00185a	journal	January 2017
Stepwise syntheses and supramolecular assemblies of a series of polyoxovanadate hybrids with various architectures Huang, Bo; Wang, Nan; Yang, Kang New Journal of Chemistry, Vol. 42, Issue 8 https://doi.org/10.1039/c7nj04727d	journal	January 2018
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Shining a light on the photo-sensitisation of organic–inorganic hybrid polyoxometalates Cameron, Jamie M.; Wales, Dominic J.; Newton, Graham N. Dalton Transactions, Vol. 47, Issue 15 https://doi.org/10.1039/c8dt00400e	journal	January 2018
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Multi-component supramolecular gels induce protonation of a porphyrin exciplex to achieve improved collective optical properties for effective photocatalytic hydrogen generation Yang, Gengxiang; Lin, Chenxiang; Feng, Xuenan Chemical Communications, Vol. 56, Issue 4 https://doi.org/10.1039/c9cc08060k	journal	January 2020
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A pore-expanded supramolecular organic framework and its enrichment of photosensitizers and catalysts for visible-light-induced hydrogen production Yan, Meng; Liu, Xu-Bo; Gao, Zhong-Zheng Organic Chemistry Frontiers, Vol. 6, Issue 10 https://doi.org/10.1039/c9qo00382g	journal	January 2019
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In Situ Loading and Delivery of Short Single- and Double-Stranded DNA by Supramolecular Organic Frameworks Yang, Bo; Zhang, Xiao-Dan; Li, Jian CCS Chemistry, Vol. 1, Issue 2 https://doi.org/10.31635/ccschem.019.20180011	journal	January 2019
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