Carbon-Carbon Bond Formation in the Electrochemical Reduction of Carbon Dioxide Catalyzed by a Ruthenium Complex

Nagao, Hidemi; Mizukawa, Tetsunori; Tanaka, Koji

doi:10.1021/ic00093a033

Cited by 173 publications

(107 citation statements)

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100

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“…However, Tanaka and co-workers reported the formation of glycolate (HOCH 2 COO-), glyoxylate (OCHCOO-), formic acid, formaldehyde, and methanol as CO 2 reduction products using [Ru(tpy)(bpy)-(CO)] 2+ complexes as electrocatalysts (bpy ) 2,2′-bipyridine, and tpy ) 2,2′:6′,2′′-terpyridine). 166 Although turnover numbers were not given for these more highly reduced species, their formation raises the exciting possibility that a single-site catalyst can result in multielectron reductions of CO 2 and even C-C bond formation. Tanaka 167 and Gibson 168 recently succeeded in isolating key Ru C 1 compounds with polypyridine ligands that are models for catalytic intermediates.…”

Section: E Electrochemical Reduction Of Comentioning

confidence: 99%

Catalysis Research of Relevance to Carbon Management: Progress, Challenges, and Opportunities

et al. 2001

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Section: E Electrochemical Reduction Of Comentioning

confidence: 99%

Catalysis Research of Relevance to Carbon Management: Progress, Challenges, and Opportunities

et al. 2001

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“…Progress has also been made on catalytic reduction of CO 2 to CO (26)(27)(28)(29)(30)(31)(32)(33)(34)(35)(36). Both present a formidable challenge in chemical reactivity.…”

mentioning

confidence: 99%

Splitting CO ₂ into CO and O ₂ by a single catalyst

Chen

Concepcion

Brennaman

et al. 2012

Proc. Natl. Acad. Sci. U.S.A.

175

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The metal complex ½ðtpyÞðMebim-pyÞRu II ðSÞ 2þ (tpy ¼ 2,2 0 : 6 0 ,2 0 0 -terpyridine; Mebim-py ¼ 3-methyl-1-pyridylbenzimidazol-2-ylidene; S ¼ solvent) is a robust, reactive electrocatalyst toward both water oxidation to oxygen and carbon dioxide reduction to carbon monoxide. Here we describe its use as a single electrocatalyst for CO 2 splitting, CO 2 → CO þ 1∕2 O 2 , in a two-compartment electrochemical cell.artificial photosynthesis | polypyridyl Ru complexes | proton coupled electron transfer | single-site catalysis | solar fuels R ising energy prices, diminishing reserves of petroleum, and environmental concerns are driving new thinking about our energy future. Given its availability, with approximately 10,000 times the daily energy input required to meet current energy consumption, solar energy could be the ultimate answer. However, solar energy is diffuse, spread over the earth's surface, and requires vast collection areas for large-scale applications (1). A more difficult challenge is the intermittency of the sun as an energy source. Meeting the challenge of providing power at night will require energy storage on massive scales at levels exceeding the ability of existing or foreseeable energy storage technologies (2, 3). The only realistic alternative is energy storage in chemical bonds and the increasingly popular concept of "solar fuels." Solar fuels mimic natural photosynthesis in using solar energy and artificial photosynthesis to convert readily available sources, water and carbon dioxide, into highenergy fuels. Target reactions include water splitting into hydrogen and oxygen and reduction of carbon dioxide to carbon monoxide, other oxygenates, or hydrocarbons (Eqs. 1-3), as follows:Carrying out these reactions presents a major challenge in chemical reactivity given their multiphoton, multielectron, multiatom character. It is reassuring that similar hurdles have been overcome in natural photosynthesis, in which light-driven reduction of CO 2 to carbohydrates by water occurs (Eq. 4). However, photosynthesis in green plants took 2-3 billion years to evolve and utilizes a complex architecture that utilizes thousands and thousands of atoms and multiple integrated assemblies (4, 5).A simplifying factor, suggesting a mechanistic approach, comes with recognition that the target energy storage reactions can be split into constituent "half reactions" which are shown for CO 2 splitting in Eqs. 5 and 6. Photosynthesis in green plants occurs in the thylakoid membrane and uses physically separated molecular assemblies for light-driven water oxidation (Photosystem II) and CO 2 reduction (Photosystem I and the Calvin cycle) (6, 7). Electron/proton equilibration occurs by intra-or transmembrane electron/proton transfer channels driven by free energy gradients.Application of a "half-reaction" strategy in artificial photosynthesis poses similar challenges. In both water oxidation and CO 2 reduction, mechanisms involving one-electron reactions are energetically untenable. They result in • OH on oxidation or CO 2•− o...

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“…159 In the homogeneous electrochemical reduction of CO 2 , a few additional C 2 species have been reported as minor products. 190 Stoichiomertic In summary, this type of system will allow us not only to investigate excited-state, proton-coupled-electron transfer reactions with a number of reductive quenchers that can also provide protons, but also to explore potential catalytic hydride transfer reactions from the hydrogenated product.…”

Section: Comparison Of the Tanaka Catalyst With The Blue Dimermentioning

confidence: 99%

Catalytic Reactions Using Transition-Metal-Complexes Toward Solar Fuel Generation

Fujita

Muckerman

2008

Bull. Jpn. Soc. Coord. Chem.

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Carbon-Carbon Bond Formation in the Electrochemical Reduction of Carbon Dioxide Catalyzed by a Ruthenium Complex

Cited by 173 publications

References 0 publications

Catalysis Research of Relevance to Carbon Management: Progress, Challenges, and Opportunities

Catalysis Research of Relevance to Carbon Management: Progress, Challenges, and Opportunities

Splitting CO ₂ into CO and O ₂ by a single catalyst

Catalytic Reactions Using Transition-Metal-Complexes Toward Solar Fuel Generation

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Carbon-Carbon Bond Formation in the Electrochemical Reduction of Carbon Dioxide Catalyzed by a Ruthenium Complex

Cited by 173 publications

References 0 publications

Catalysis Research of Relevance to Carbon Management: Progress, Challenges, and Opportunities

Catalysis Research of Relevance to Carbon Management: Progress, Challenges, and Opportunities

Splitting CO 2 into CO and O 2 by a single catalyst

Catalytic Reactions Using Transition-Metal-Complexes Toward Solar Fuel Generation

Contact Info

Product

Resources

About

Splitting CO ₂ into CO and O ₂ by a single catalyst