CO<sub>2</sub> Capture by a Rhenium(I) Complex with the Aid of Triethanolamine

Morimoto, Tatsuki; Nakajima, Takehiko; Sawa, Shuhei; Nakanishi, Ryoichi; Imori, Daisuke; Ishitani, Osamu

doi:10.1021/ja409271s

Cited by 228 publications

(287 citation statements)

References 25 publications

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“…60 It is unknown whether or not TEOA coordinates to the Mn center during this process; however, previous studies with Re bipyridine photocatalysts have shown that CO 2 can bind to the metal center with the aid of TEOA, forming an O-bound Re−OC(O)OCH 2 CH 2 NR 2 complex. 61 68 In the original report of the photocatalytic ability of Mn(bpy)(CO) 3 Br by Takeda et al in 2014, the authors report slightly lower TONs for formate by only the Ru 2+ photosensitizer (TON = 25 after 12 h). 45 Although the [Ru(dmb) 3 ] 2+ photosensitizer also serves as a catalyst for CO 2 reduction, it is clear that the Mn complex enhances CO 2 reduction to formate by at least a factor of ∼2 in the homogeneous system and a factor of ∼3 in the heterogeneous UiO-67-Mn(bpy)(CO) 3 Br system.…”

Section: ■ Results and Discuissonmentioning

confidence: 99%

Photocatalytic CO₂Reduction to Formate Using a Mn(I) Molecular Catalyst in a Robust Metal–Organic Framework

et al. 2015

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A manganese bipyridine complex, Mn(bpydc)(CO)3Br (bpydc = 5,5'-dicarboxylate-2,2'-bipyridine), has been incorporated into a highly robust Zr(IV)-based metal-organic framework (MOF) for use as a CO2 reduction photocatalyst. In conjunction with [Ru(dmb)3](2+) (dmb = 4,4'-dimethyl-2,2'-bipyridine) as a photosensitizer and 1-benzyl-1,4-dihydronicotinamide (BNAH) as a sacrificial reductant, Mn-incorporated MOFs efficiently catalyze CO2 reduction to formate in DMF/triethanolamine under visible-light irradiation. The photochemical performance of the Mn-incorporated MOF reached a turnover number of approximately 110 in 18 h, exceeding that of the homogeneous reference systems. The increased activity of the MOF-incorporated Mn catalyst is ascribed to the struts of the framework providing isolated active sites, which stabilize the catalyst and inhibit dimerization of the singly reduced Mn complex. The MOF catalyst largely retained its crystallinity throughout prolonged catalysis and was successfully reused over several catalytic runs.

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Section: ■ Results and Discuissonmentioning

confidence: 99%

Photocatalytic CO₂Reduction to Formate Using a Mn(I) Molecular Catalyst in a Robust Metal–Organic Framework

et al. 2015

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“…Consequently, every study focusses on hydrogen evolution by means of a sacrificial electron donor (usually triethanolamine or trimethylamine) to provide an oxidative half reaction to close the catalytic cycle. It is vital to understand the role of these sacrificial electron donors 78 such that we can replace them by recyclable electron donors. 79,80 Then, by combining this system with a water oxidation catalyst, sustainable solar fuel generation can be achieved.…”

Section: Discussionmentioning

confidence: 99%

Understanding metal–organic frameworks for photocatalytic solar fuel production

et al. 2017

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The fascinating chemical and physical properties of MOFs have recently stimulated exploration of their application for photocatalysis. Despite the intense research effort, the efficiency of most photocatalytic MOFs for solar fuel generation is still very modest. In this highlight we analyse the current status of the field and stress the potential of advanced spectroscopic techniques to gain structural and mechanistic insight and hence support the future development of MOFs to harvest and store solar energy.

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“…This may suggest the necessary involvement of TEOA as both a sacrificial electron and proton donor in the photocatalyzed reaction. [22] Under the same CO 2 photocatalytic conditions as that of the TiO 2 -rGO-Re(PyBn)(CO) 3 Cl composite, TiO 2 nanoparticles produced no measurable CO or CH 4 ; this differs from the TiO 2 -catalyzed photo-reduction of CO 2 to produce CH 4 using 2-propanol as a sacrificial donor. [23] The photo-stability of the catalyst composite was then evaluated.…”

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confidence: 94%

Photo‐reduction of CO₂ Using a Rhenium Complex Covalently Supported on a Graphene/TiO₂ Composite

2016

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One of the promising solutions for decreasing atmospheric CO2 is artificial photosynthesis, in which CO2 can be photoconverted into solar fuels. In this study, a rhenium complex Re(PyBn)(CO)3 Cl (PyBn=1-(2-picolyl)-4-phenyl-1H-1,2,3-triazole) was covalently grafted onto the surface of reduced graphene oxide (rGO). This was further combined with TiO2 to fabricate a novel catalyst composite TiO2 -rGO-Re(PyBn)(CO)3 Cl for CO2 photo-reduction. This hybrid composite demonstrated high selectivity conversion of CO2 into CO under xenon-lamp irradiation. Compared with the unsupported homogeneous catalyst Re(PyBn)(CO)3 Cl, the covalent immobilized catalyst composite TiO2 -rGO-Re(PyBn)(CO)3 Cl enhanced the turnover number six times and significantly improved catalyst stability. During the process of CO2 photo-reduction, intermediate species with lifetimes longer than hundreds of microseconds were observed and the formation of CO products was revealed using timeresolved infrared spectroscopy. A plausible mechanism for CO2 photo-reduction by the TiO2 -rGO-Re(PyBn)(CO)3 Cl catalyst composite has been suggested. The obtained results have implications for the future design of efficient catalyst composites for CO2 photo-conversion.

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CO₂ Capture by a Rhenium(I) Complex with the Aid of Triethanolamine

Cited by 228 publications

References 25 publications

Photocatalytic CO₂Reduction to Formate Using a Mn(I) Molecular Catalyst in a Robust Metal–Organic Framework

Photocatalytic CO₂Reduction to Formate Using a Mn(I) Molecular Catalyst in a Robust Metal–Organic Framework

Understanding metal–organic frameworks for photocatalytic solar fuel production

Photo‐reduction of CO₂ Using a Rhenium Complex Covalently Supported on a Graphene/TiO₂ Composite

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CO2 Capture by a Rhenium(I) Complex with the Aid of Triethanolamine

Cited by 228 publications

References 25 publications

Photocatalytic CO2Reduction to Formate Using a Mn(I) Molecular Catalyst in a Robust Metal–Organic Framework

Photocatalytic CO2Reduction to Formate Using a Mn(I) Molecular Catalyst in a Robust Metal–Organic Framework

Understanding metal–organic frameworks for photocatalytic solar fuel production

Photo‐reduction of CO2 Using a Rhenium Complex Covalently Supported on a Graphene/TiO2 Composite

Contact Info

Product

Resources

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CO₂ Capture by a Rhenium(I) Complex with the Aid of Triethanolamine

Photocatalytic CO₂Reduction to Formate Using a Mn(I) Molecular Catalyst in a Robust Metal–Organic Framework

Photocatalytic CO₂Reduction to Formate Using a Mn(I) Molecular Catalyst in a Robust Metal–Organic Framework

Photo‐reduction of CO₂ Using a Rhenium Complex Covalently Supported on a Graphene/TiO₂ Composite