Light driven styrene epoxidation and hydrogen generation using H2O as an oxygen source in a photoelectrosynthesis cellElectronic supplementary information (ESI) available: Experimental section containing the preparation of photoanodes and modified membranes, cell construction and additional spectroscopic, electrochemical, and catalytic data. See DOI: 10.1039/c5gc01589h

A dye-sensitized photoelectrosynthesis cell (DSPEC) has been prepared for the oxidation of alkenes to epoxides and evolution of hydrogen using water as an oxygen source and sunlight. A Ru oxidation catalyst, 2,2 + , is used in the homogeneous phase in the anodic compartment to oxidize a water-solubl...

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Hauptverfasser: Farràs, P, Di Giovanni, C, Clifford, J. N, Garrido-Barros, P, Palomares, E, Llobet, A
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Zusammenfassung:A dye-sensitized photoelectrosynthesis cell (DSPEC) has been prepared for the oxidation of alkenes to epoxides and evolution of hydrogen using water as an oxygen source and sunlight. A Ru oxidation catalyst, 2,2 + , is used in the homogeneous phase in the anodic compartment to oxidize a water-soluble alkene, 4-styrene sulfonic acid (4-HSS), to the corresponding epoxide that in acidic solution is hydrolyzed to the diol (4-(1,2-dihydroxyethyl)-benzenesulfonic acid). Concomitantly, protons are generated that diffuse through a proton exchange membrane to a Pt cathode where they are transformed into hydrogen. Illumination under 1.5 AMG (100 mW cm −2 ) together with an external bias of 0.3 V vs. NHE after 24 h leads to the generation of 1.28 Coulombs together with the formation of 6.1 μmol of H 2 at the cathodic compartment that corresponds to a faradaic efficiency of 92%. In addition 0.7 mM of the 4-HSS substrate has been oxidized at the anodic compartment with a conversion yield of 7%. The rate of hydrogen evolution is limited by the oxidation of the organic substrate, and the TOF for both reactions is measured to be 0.8 ks −1 . This proof-of-concept dye-sensitized photoelectrosynthesis cell is able to produce a high-value chemical by the epoxidation of an alkene in water using sunlight and, at the same time, produce a solar fuel such as hydrogen.
ISSN:1463-9262
1463-9270
DOI:10.1039/c5gc01589h