PHOTOCHEMICAL CO2 REDUCTION BY RHENUIM AND RUTHENIUM COMPLEXES.

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Photochemical conversion of CO{sub 2} to fuels or useful chemicals using renewable solar energy is an attractive solution to both the world's need for fuels and the reduction of greenhouse gases. Rhenium(I) and ruthenium(II) diimine complexes have been shown to act as photocatalysts and/or electrocatalysts for CO{sub 2} reduction to CO. We have studied these photochemical systems focusing on the identification of intermediates and the bond formation/cleavage reactions between the metal center and CO{sub 2}. For example, we have produced the one-electron-reduced monomer (i.e. Re(dmb)(CO){sub 3}S where dmb = 4,4'-dimethy-2,2'-bipyridine and S = solvent) either by reductive quenching of the ... continued below

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FUJITA,E.; MUCKERMAN, J.T. & TANAKA, K. November 30, 2007.

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Photochemical conversion of CO{sub 2} to fuels or useful chemicals using renewable solar energy is an attractive solution to both the world's need for fuels and the reduction of greenhouse gases. Rhenium(I) and ruthenium(II) diimine complexes have been shown to act as photocatalysts and/or electrocatalysts for CO{sub 2} reduction to CO. We have studied these photochemical systems focusing on the identification of intermediates and the bond formation/cleavage reactions between the metal center and CO{sub 2}. For example, we have produced the one-electron-reduced monomer (i.e. Re(dmb)(CO){sub 3}S where dmb = 4,4'-dimethy-2,2'-bipyridine and S = solvent) either by reductive quenching of the excited states of fac-[Re(dmb)(CO){sub 3}(CH{sub 3}CN)]PF{sub 6} or by photo-induced homolysis of [Re(dmb)(CO){sub 3}]{sub 2}. We previously found that: (1) the remarkably slow dimerization of Re(dmb)(CO){sub 3}S is due to the absence of a vacant coordination site for Re-Re bond formation, and the extra electron is located on the dmb ligand; (2) the reaction of Re(dmb)(CO){sub 3}S with CO{sub 2} forms a CO{sub 2}-bridged binuclear species (CO){sub 3}(dmb)Re-CO(O)-Re(dmb)(CO){sub 3} as an intermediate in CO formation; and (3) the kinetics and mechanism of reactions are consistent with the interaction of the CO{sub 2}-bridged binuclear species with CO{sub 2} to form CO and CO{sub 3}{sup 2-}.

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  • 235TH ACS NATIONAL MEETING; NEW ORLEANS, LA; 20080406 through 20080410

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  • Report No.: BNL--79593-2007-CP
  • Grant Number: DE-AC02-98CH10886
  • Office of Scientific & Technical Information Report Number: 925820
  • Archival Resource Key: ark:/67531/metadc894585

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  • November 30, 2007

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  • Sept. 27, 2016, 1:39 a.m.

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  • Nov. 1, 2016, 5 p.m.

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FUJITA,E.; MUCKERMAN, J.T. & TANAKA, K. PHOTOCHEMICAL CO2 REDUCTION BY RHENUIM AND RUTHENIUM COMPLEXES., article, November 30, 2007; United States. (digital.library.unt.edu/ark:/67531/metadc894585/: accessed October 16, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.