Molecular Cobalt Clusters as Precursors of Distinct Active Species in Electrochemical, Photochemical, and Photoelectrochemical Water Oxidation Reactions in Phosphate Electrolytes

Three cobalt model molecular compounds, Co‐cubane ([Co4(µ3‐O)4(µ‐OAc)4py4]), Co‐trimer ([Co3(μ3‐O)(µ‐OAc)6py3]PF6), and Co‐dimer ([Co2(μ‐OH)2(µ‐OAc)(OAc)2py4]PF6), are investigated as water oxidation reaction (WOR) catalysts, using electrochemical, photochemical, and photoelectrochemical methodologi...

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Vydáno v:	Chemistry : a European journal Ročník 21; číslo 46; s. 16578 - 16584
Hlavní autoři:	Li, Xiaobo, Clatworthy, Edwin B., Masters, Anthony F., Maschmeyer, Thomas
Médium:	Journal Article
Jazyk:	angličtina
Vydáno:	Weinheim WILEY-VCH Verlag 09.11.2015 WILEY‐VCH Verlag Wiley Subscription Services, Inc
Témata:	Carbon dioxide Catalysis Catalysts Catalytic activity Chemical reactions Chemistry Cobalt Cobalt compounds cobalt oxide Cubane Dimers Electrochemistry Electrolytes Oxidation oxygen evolution Photochemical Photochemicals Precursors Species Trimers water oxidation cobalt electrochemistry water oxidation oxygen evolution cobalt oxide cubane
ISSN:	0947-6539, 1521-3765
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Shrnutí:	Three cobalt model molecular compounds, Co‐cubane ([Co4(µ3‐O)4(µ‐OAc)4py4]), Co‐trimer ([Co3(μ3‐O)(µ‐OAc)6py3]PF6), and Co‐dimer ([Co2(μ‐OH)2(µ‐OAc)(OAc)2py4]PF6), are investigated as water oxidation reaction (WOR) catalysts, using electrochemical, photochemical, and photoelectrochemical methodologies in phosphate electrolyte. The actual species contributing to the catalytic activity observed in the WOR are derived from the transformation of these cobalt compounds. The catalytic activity observed is highly dependent on the initial compound structure and on the particular WOR methodology used. Co‐cubane shows no activity in the electrochemical WOR and negligible activity in the photochemical WOR, but is active in the photoelectrochemical WOR, in which it behaves as a precursor to catalytically active species. Co‐dimer also shows no activity in the electrochemical WOR, but behaves as a precursor to catalytically active species in both the photochemical and photoelectrochemical WOR experiments. Co‐trimer behaves as a precursor to catalytically active species in all three of the WOR methodologies. Cobalt catalysts: The cobalt species derived in situ from the three molecular cobalt compounds, Co‐cubane, Co‐trimer, and Co‐dimer, are found to be the actual catalytic species for the observed water oxidation activity in three water oxidation methodologies (electrochemical, photochemical, and photoelectrochemical). However, the ability to form active species from the cobalt precursors is highly dependent on their structure and the water oxidation reaction (WOR) protocols, as shown in the figure.
Bibliografie:	ArticleID:CHEM201502428 ark:/67375/WNG-0DCP562R-6 istex:CDC75104AA3F6FC3F54FAF00B20AC69BA469A27F Australian Research Council ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 14 content type line 23
ISSN:	0947-6539 1521-3765
DOI:	10.1002/chem.201502428