Dataset Information

A visible-light harvesting system for CO2 reduction using a Ru(II) -Re(I) photocatalyst adsorbed in mesoporous organosilica.

ABSTRACT: A photocatalytic system for CO2 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 CO2 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.

SUBMITTER: Ueda Y

PROVIDER: S-EPMC4544448 | biostudies-literature | 2015 Feb

REPOSITORIES: biostudies-literature

ACCESS DATA

Publications

A visible-light harvesting system for CO2 reduction using a Ru(II) -Re(I) photocatalyst adsorbed in mesoporous organosilica.

Ueda Yutaro Y Takeda Hiroyuki H Yui Tatsuto T Koike Kazuhide K Goto Yasutomo Y Inagaki Shinji S Ishitani Osamu O

ChemSusChem 20141218 3

A photocatalytic system for CO2 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 ex ...[more]

PMID: 25524162

Similar Datasets

Project description:We have designed and synthesized a new tris-chelating polypyridine ligand (bpy3Ph) suitable to be used as a bridging ligand (BL) for constructing various supramolecular photocatalysts. This BL is a phenylene ring with three ethylene chains at 1, 3, and 5 positions, of which the other terminals are connected to 2,2'-bipyridine moieties. The ligand bpy3Ph has been used to prepare, according to a multi-step synthetic protocol, trinuclear supramolecular photocatalysts containing different metal subunits. In particular, the compounds Ru2Re and RuRe2 have been prepared, containing different ratios of components based on Ru(dmb)3 2+-type and Re(dmb)(CO)3Cl-type units (dmb = 4,4'-dimethyl-2,2'-bipyridine), which can play the roles of photosensitizers and catalyst units for photocatalytic CO2 reduction, respectively. The trinuclear model Ru3 and mononuclear and dinuclear Ru and Ru2 precursor metal complexes, containing free chelating sites, have also been synthesized using the same bridging ligand. The absorption spectra, redox behaviour and photophysical properties of the new species indicate that there is no strong electronic interaction among the Ru and Re units. The trinuclear complexes Ru2Re and RuRe2 could photocatalyze CO2 reduction to CO with high selectivity (up to 97%), high efficiency (Φ COs of 28% and 25%, respectively: BIH as a reductant), and high durability (TONCOs of 5232 and 6038, respectively: BIH as a reductant) which are the largest TONs for CO2 reduction using supramolecular photocatalysts in homogeneous solutions. The absence of negligible accumulation of the mono-reduced form of the photosensitizer indicates fast electron transfer to the catalyst unit(s) through the relatively large bridging ligand and is proposed to contribute to the outstanding photocatalytic properties of the new species, including their durability. The relevant photocatalytic behaviour of the new systems indicates new avenues for the design of extended bridging ligands capable of efficiently and functionally integrating photosensitizers and catalysts towards the preparation of new, larger supramolecular photocatalysts for selective CO2 reduction.

Dataset Information

A visible-light harvesting system for CO2 reduction using a Ru(II) -Re(I) photocatalyst adsorbed in mesoporous organosilica.

Publications

A visible-light harvesting system for CO2 reduction using a Ru(II) -Re(I) photocatalyst adsorbed in mesoporous organosilica.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets