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

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms11580· OSTI ID:1379333
 [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

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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1379333
Journal Information:
Nature Communications, Vol. 7; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 159 works
Citation information provided by
Web of Science

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Water‐Soluble Conjugated Molecule for Solar‐Driven Hydrogen Evolution from Salt Water journal February 2019
Modular Assembly of Host–Guest Metal–Phenolic Networks Using Macrocyclic Building Blocks journal November 2019
Shape-Controllable and Fluorescent Supramolecular Organic Frameworks Through Aqueous Host-Guest Complexation journal December 2017
Modular Assembly of Host–Guest Metal–Phenolic Networks Using Macrocyclic Building Blocks journal November 2019
2:2 Complexes from Diphenylpyridiniums and Cucurbit[8]uril: Encapsulation-Promoted Dimerization of Electrostatically Repulsing Pyridiniums journal April 2018
Highly Luminescent and Water-Soluble Two-Dimensional Supramolecular Organic Framework: All-Organic Photosensitizer Template for Visible-Light-Driven Hydrogen Evolution from Water journal January 2018
Photocatalytic Decontamination of Wastewater Containing Organic Dyes by Metal-Organic Frameworks and their Derivatives journal October 2016
Outer Surface Interactions of Cucurbit[6]uril That Trigger the Assembly of Supramolecular Three-Dimensional Polycatenanes journal January 2017
Engineering Metal–Organic Framework Catalysts for C−C and C−X Coupling Reactions: Advances in Reticular Approaches from 2014–2018 journal September 2019
Cucurbit[7]uril‐Based Metal–Organic Rotaxane Framework for Dual‐Capture of Molecular Iodine and Cationic Potassium Ion journal January 2020
Metal-Organic-Framework-Derived Co 3 S 4 Hollow Nanoboxes for the Selective Reduction of Nitroarenes journal August 2018
Orthogonal Supramolecular Assembly Triggered by Inclusion and Exclusion Interactions with Cucurbit[7]uril for Photocatalytic H 2 Evolution journal December 2019
Physical and Electrochemical Modulation of Polyoxometalate Ionic Liquids via Organic Functionalization: Physical and Electrochemical Modulation of Polyoxometalate Ionic Liquids via Organic Functionalization journal August 2018
Supramolecular Chemistry in Solid State Materials such as Metal-Organic Frameworks journal October 2018
Supramolecular Polymerization from Controllable Fabrication to Living Polymerization journal July 2017
Metal Organic Frameworks: A New Generation Coordination Polymers for Visible Light Photocatalysis journal July 2017
Photolysis Behaviors of Anthryl Derivative Aggregation Mediated by Sulfato‐β‐Cyclodextrin journal December 2019
Enhancing Hydrogen Generation Through Nanoconfinement of Sensitizers and Catalysts in a Homogeneous Supramolecular Organic Framework journal May 2018
Maximizing the photocatalytic hydrogen evolution of Z-scheme UiO-66-NH2@Au@CdS by aminated-functionalized linkers journal February 2019
A stable metal-covalent-supramolecular organic framework hybrid: enrichment of catalysts for visible light-induced hydrogen production journal April 2018
Controllable macrocyclic supramolecular assemblies in aqueous solution journal July 2018
Anion-adaptive crystalline cationic material for 99TcO4− trapping journal April 2019
Fluorescence enhancement through the formation of a single-layer two-dimensional supramolecular organic framework and its application in highly selective recognition of picric acid journal January 2016
Surveying macrocyclic chemistry: from flexible crown ethers to rigid cyclophanes journal January 2017
Stepwise syntheses and supramolecular assemblies of a series of polyoxovanadate hybrids with various architectures journal January 2018
C–C to CC conversion within a supramolecular framework of tetrathiafulvalene: a confinement effect and an oxygen related dehydrogenation journal January 2018
From double-shelled grids to supramolecular frameworks journal January 2018
Synergistic catalysis for light-driven proton reduction using a polyoxometalate-based Cu–Ni heterometallic–organic framework journal January 2019
Shining a light on the photo-sensitisation of organic–inorganic hybrid polyoxometalates journal January 2018
Visible-light initiated aerobic oxidations: a critical review journal January 2018
Fabrication of nor-seco -cucurbit[10]uril based supramolecular polymers via self-sorting journal January 2019
Multi-component supramolecular gels induce protonation of a porphyrin exciplex to achieve improved collective optical properties for effective photocatalytic hydrogen generation journal January 2020
Triptycene walled glycoluril trimer: synthesis and recognition properties journal January 2020
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In Situ Loading and Delivery of Short Single- and Double-Stranded DNA by Supramolecular Organic Frameworks journal January 2019
Supramolecular Chemistry and Self-Organization: A Veritable Playground for Catalysis journal February 2019
Shape‐Controllable and Fluorescent Supramolecular Organic Frameworks Through Aqueous Host–Guest Complexation journal December 2017
A study of binding interactions between terpyridine derivatives and cucurbit[10]uril text January 2018
A study of binding interactions between terpyridine derivatives and cucurbit[10]uril text January 2018