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      A Visible-Light Harvesting System for CO 2 Reduction Using a Ru II–Re I Photocatalyst Adsorbed in Mesoporous Organosilica

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          A photocatalytic system for CO 2 reduction exhibiting visible-light harvesting was developed by preparing a hybrid consisting of a supramolecular metal complex as photocatalyst and periodic mesoporous organosilica (PMO) as light harvester. A Ru II–Re I binuclear complex (Ru–Re) with methylphosphonic acid anchor groups was adsorbed on acridone or methylacridone embedded in the walls of PMO mesochannels to yield the hybrid structure. The embedded organic groups absorbed visible light, and the excitation energy was funneled to the Ru units. The energy accumulation was followed by electron transfer and catalytic reduction of CO 2 to CO on the Re unit. The light harvesting of these hybrids enhanced the photocatalytic CO evolution rate by a factor of up to ten compared with that of Ru–Re adsorbed on mesoporous silica without a light harvester.

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          Most cited references 17

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          Energy transfer dynamics in metal-organic frameworks.

          Isomorphous metal-organic frameworks (MOFs) based on {M[4,4'-(HO(2)C)(2)-bpy](2)bpy}(2+) building blocks (where M = Ru or Os) were designed and synthesized to study the classic Ru to Os energy transfer process that has potential applications in light-harvesting with supramolecular assemblies. The crystalline nature of the MOFs allows precise determination of the distances between metal centers by X-ray diffraction, thereby facilitating the study of the Ru→Os energy transfer process. The mixed-metal MOFs with 0.3, 0.6, 1.4, and 2.6 mol % Os doping were also synthesized in order to study the energy transfer dynamics with a two-photon excitation at 850 nm. The Ru lifetime at 620 nm decreases from 171 ns in the pure Ru MOF to 29 ns in the sample with 2.6 mol % Os doping. In the mixed-metal samples, energy transfer was observed with an initial growth in Os emission corresponding with the rate of decay of the Ru excited state. These results demonstrate rapid, efficient energy migration and long distance transfer in isomorphous MOFs.
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            Enhanced photocatalysis of rhenium(I) complex by light-harvesting periodic mesoporous organosilica.

            This paper describes a new conceptual design for enhancement of photocatalytic CO(2) reduction of a rhenium(I) complex by light harvesting of periodic mesoporous organosilica (PMO). Mesoporous biphenyl-silica (Bp-PMO) anchoring fac-[Re(I)(bpy)(CO)(3)(PPh(3))](+)(OTf)(-) (bpy =2,2'-bipyridine; OTf = CF(3)SO(3)) in the mesochannels was synthesized by co-condensation of two organosilane precursors, 4,4'-bis(triethoxysilyl)biphenyl and 4-[4-{3-(trimethoxysilyl)propylsulfanyl}butyl]-4'-methyl-2,2'-bipyridine in the presence of a template surfactant, followed by coordination of a rhenium precursor, [Re(I)(CO)(5)(PPh(3))](+)(OTf)(-) to the bipyridine ligand in the mesochannels. The 280 nm light was effectively absorbed by the biphenyl groups in Bp-PMO, and the excited energy was funneled into the Re complex by resonance energy transfer, which enhanced photocatalytic CO evolution from CO(2) by a factor of 4.4 compared with direct excitation of the Re complex. Bp-PMO had an additional merit to protect the Re complex against a decomposition by UV irradiation. These results demonstrate the potential of PMOs as a light-harvesting antenna for designing various photoreaction systems, mimicking the natural photosynthesis.
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              A compact diketopyrrolopyrrole dye as efficient sensitizer in titanium dioxide dye-sensitized solar cells


                Author and article information

                WILEY-VCH Verlag (Weinheim )
                February 2015
                18 December 2014
                : 8
                : 3
                : 439-442
                [[a] ]Department of Chemistry, Graduate School of Science and Engineering, Tokyo Institute of Technology 2-12-1-NE-1 O-okayama, Meguro-ku, Tokyo 152-8550 (Japan) E-mail: ishitani@ 123456chem.titech.ac.jp
                [[b] ]Toyota Central R&D Labs. Inc. Yokomichi Nagakute, Aichi 480-1192 (Japan) E-mail: inagaki@ 123456mosk.tytlabs.co.jp
                [[c] ]Department of Materials Science and Technology, Faculty of Engineering, Niigata University 8050 Ikarashi-2, Niigata 950-2181 (Japan)
                [[d] ]National Institute of Advanced Industrial Science and Technology 16-1 Onogawa, Tsukuba 305-8569 (Japan)
                Author notes

                Supporting Information for this article is available on the WWW under http://dx.doi.org/10.1002/cssc.201403194.

                © 2015 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution Non-Commercial License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes.


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