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A Molecular Z-Scheme Artificial Photosynthetic System Under the Bias-Free Condition for CO2 Reduction Coupled with Two-electron Water Oxidation: Photocatalytic Production of CO/HCOOH and H2O2 |
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| Authors: | Dr Fazalurahman Kuttassery Yutaka Ohsaki Dr Arun Thomas Ryutaro Kamata Yosuke Ebato Dr Hiromu Kumagai Ryosuke Nakazato Dr Abin Sebastian Dr Siby Mathew Prof Hiroshi Tachibana Prof Osamu Ishitani Prof Haruo Inoue |
| Institution: | 1. Department of Chemistry, University of Calicut, Malappuram, Kerala, 673635 India;2. Department of Applied Chemistry for Environment, Graduate School of Urban Environmental Sciences, Tokyo Metropolitan University, 1-1 Minami Osawa, Hachioji, Tokyo, 192-0397 Japan;3. Department of Chemistry, St. Stephen's College, Uzhavoor, Kerala, 686634 India;4. Department of Chemistry, Tokyo Institute of Technology, 2-12-1-NE-1 O-okayama, Meguro, Tokyo, 152-8550 Japan;5. Research Center for Advanced Science and Technology, The University of Tokyo, 4-6-1 Komaba, Meguro, Tokyo, 153-8904 Japan |
| Abstract: | Bio-inspired molecular-engineered systems have been extensively investigated for the half-reactions of H2O oxidation or CO2 reduction with sacrificial electron donors/acceptors. However, there has yet to be reported a device for dye-sensitized molecular photoanodes coupled with molecular photocathodes in an aqueous solution without the use of sacrificial reagents. Herein, we will report the integration of SnIV- or AlIII-tetrapyridylporphyrin (SnTPyP or AlTPyP) decorated tin oxide particles (SnTPyP/SnO2 or AlTPyP/SnO2) photoanode with the dye-sensitized molecular photocathode on nickel oxide particles containing Ru(diimine)3]2+ as the light-harvesting unit and Ru(diimine)(CO)2Cl2] as the catalyst unit covalently connected and fixed within poly-pyrrole layer (RuCAT-RuC2-PolyPyr-PRu/NiO). The simultaneous irradiation of the two photoelectrodes with visible light resulted in H2O2 on the anode and CO, HCOOH, and H2 on the cathode with high Faradaic efficiencies in purely aqueous conditions without any applied bias is the first example of artificial photosynthesis with only two-electron redox reactions. |
| Keywords: | CO2 Reduction Photocatalytic Reactions Photoelectrochemical Cell Selective Formation of H2O2 Water Oxidation |