Photoelectrochemical CO<sub>2</sub> reduction using a Ru(<scp>ii</scp>)–Re(<scp>i</scp>) multinuclear metal complex on a p-type semiconducting NiO electrode

Sahara, Go; Abe, Ryu; Higashi, Masanobu; Morikawa, Takeshi; Maeda, Kazuhiko; Ueda, Yutaro; Ishitani, Osamu

doi:10.1039/c5cc02403j

Cited by 132 publications

(122 citation statements)

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“…[46] Figure S1 shows the UV/Vis absorption spectrum of RuRe in acetonitrile (MeCN), along with its model mononuclear complexes of Ru and Re(dmb)(CO) 3 Br (dmb = 4,4'-dimethyl-2,2'-bipyridine). [47] Electrochemical measurements were obtainedf or RuRe in aD MA/TEOA (triethanolamine)s olutionu nder an Ar (Figure S2 Ai nt he Supporting Information) or CO 2 atmosphere (Figure S2 B). In contrast, the Re complex produced aw eak absorption band in the visible-lightr egion.…”

Section: Resultsmentioning

confidence: 99%

Activation of the Carbon Nitride Surface by Silica in a CO‐Evolving Hybrid Photocatalyst

et al. 2016

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Photocatalytic reduction of CO2 to CO proceeded by visible light (λ>400 nm) using mesoporous graphitic carbon nitride (C3N4) coupled with a RuII–ReI binuclear complex (RuRe) containing a photosensitizer and catalytic units. The selectivity to CO exceeded 90 % during the initial stage. Photocatalytic reactions (including isotope tracer experiments) and electrochemical measurements revealed that the reaction proceeded according to a two‐step photoexcitation of C3N4 and the RuII photosensitizer unit, that is, it followed the Z‐Scheme mechanism. Modification of C3N4 with highly dispersed silica was found to improve the ability of C3N4 to accommodate RuRe, which enhanced the photocatalytic activity for CO production.

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Section: Resultsmentioning

confidence: 99%

Activation of the Carbon Nitride Surface by Silica in a CO‐Evolving Hybrid Photocatalyst

et al. 2016

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“…These include catalysts of carbon dioxide reduction: trans(Cl)–Ru(bpy)(CO) 2 Cl 2 or Ru 58 and Re(4,4′-dimethyl-bpy)(CO) 3 Br or Re . 59 Catalysts used for hydrogen production or proton reduction catalysts: a cobalt–salen complex, 6,6′-((1E,1′E)-(ethane-1,2-diylbis(azanylylidene)) bis(methanylylidene))bis-(2,4-ditert-butylphenol)cobalt(III) or Co1 60 and [Co III (Cp*)(bpy)(OH)] 2+ where Cp* = η 5 -pentamethylcyclopentadienyl or Co2 . 61 Catalysts used for oxygen production: [Rh III (dmbpy) 2 Cl 2 + ] where dmbpy = 4,4′-dimethyl-2,2′-bipyridine or Rh , 62 (2,5-dpp)PdCl 2 with 2,5-di(pyridine-2-yl)pyrazine or Pd1 , 63 (2,6-dpp)PdCl 2 with 2,6-di(pyridine-2-yl)pyrazine or Pd2 , 64 [Co III (CR)Cl 2 ] + where CR = 2,12-dimethyl-3,7,11,17-tetra-azabicyclo (11.3.1)-heptadeca-1(17),2,11,13,15-pentaene) or Co3 , 65 and 5-[4-(5-carboxyl-2,7-di-tert-butyl-9,9-dimethylxanthene)]-10,15,20-tris(pentafluoro-phenyl)porphyrinatocobalt(I) or Co4 .…”

Section: Resultsmentioning

confidence: 99%

Computational characterization of competing energy and electron transfer states in bimetallic donor-acceptor systems for photocatalytic conversion

Fredin

Persson

2016

The Journal of Chemical Physics

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The rapidly growing interest in photocatalytic systems for direct solar fuel production, such as hydrogen generation from water splitting is grounded in the unique opportunity to achieve charge separation in molecular systems provided by electron transfer processes. In general, both photoinduced and catalytic processes involve complicated dynamics that depend on both structural and electronic effects. Here the excited state landscape of metal centered light harvester-catalyst pairs is explored using density functional theory (DFT) calculations. In weakly bound systems, the interplay between structural and electronic factors involved can be constructed from the various mononuclear relaxed excited states. For this study, supramolecular states of electron transfer and excitation energy transfer character have been constructed from constituent full optimizations of multiple charge/spin states for a set of three Ru-based light harvesters and nine transition metal catalysts (based on Ru, Rh, Re, Pd, and Co) in terms of energy, structure, and electronic properties. The complete set of combined charge-spin states for each donor-acceptor system provides information about the competition of excited state energy transfer states with the catalytically active electron transfer states, enabling the identification of the most promising candidates for photocatalytic applications from this perspective.

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“…The integration of a p-type NiO cathode with this complex induced an intrinsic improvement for CO 2 reduction to CO (Fig. 12b) [134]. The TON reached 32 with FE of 62% after reacting for 3 h, and excellent durability was achieved when the reaction was prolonged to 5 h with FE increased to 98%.…”

Section: Metal Complexesmentioning

confidence: 88%

Recent progress on advanced design for photoelectrochemical reduction of CO2 to fuels

et al. 2018

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The energy crisis and global warming become severe issues. Solar-driven CO 2 reduction provides a promising route to confront the predicaments, which has received much attention. The photoelectrochemical (PEC) process, which can integrate the merits of both photocatalysis and electrocatalysis, boosts splendid talent for CO 2 reduction with high efficiency and excellent selectivity. Recent several decades have witnessed the overwhelming development of PEC CO 2 reduction. In this review, we attempt to systematically summarize the recent advanced design for PEC CO 2 reduction. On account of basic principles and evaluation parameters, we firstly highlight the subtle construction for photocathodes to enhance the efficiency and selectivity of CO 2 reduction, which includes the strategies for improving light utilization, supplying catalytic active sites and steering reaction pathway. Furthermore, diversiform novel PEC setups are also outlined. These exploited setups endow a bright window to surmount the intrinsic disadvantages of photocathode, showing promising potentials for future applications. Finally, we underline the challenges and key factors for the further development of PEC CO 2 reduction that would enable more efficient designs for setups and deepen systematic understanding for mechanisms.

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Photoelectrochemical CO₂ reduction using a Ru(ii)–Re(i) multinuclear metal complex on a p-type semiconducting NiO electrode

Cited by 132 publications

References 13 publications

Activation of the Carbon Nitride Surface by Silica in a CO‐Evolving Hybrid Photocatalyst

Activation of the Carbon Nitride Surface by Silica in a CO‐Evolving Hybrid Photocatalyst

Computational characterization of competing energy and electron transfer states in bimetallic donor-acceptor systems for photocatalytic conversion

Recent progress on advanced design for photoelectrochemical reduction of CO2 to fuels

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Photoelectrochemical CO2 reduction using a Ru(ii)–Re(i) multinuclear metal complex on a p-type semiconducting NiO electrode

Cited by 132 publications

References 13 publications

Activation of the Carbon Nitride Surface by Silica in a CO‐Evolving Hybrid Photocatalyst

Activation of the Carbon Nitride Surface by Silica in a CO‐Evolving Hybrid Photocatalyst

Computational characterization of competing energy and electron transfer states in bimetallic donor-acceptor systems for photocatalytic conversion

Recent progress on advanced design for photoelectrochemical reduction of CO2 to fuels

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Photoelectrochemical CO₂ reduction using a Ru(ii)–Re(i) multinuclear metal complex on a p-type semiconducting NiO electrode