Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 28, Issue 10, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202102630
Keywords
heterogeneous catalysis; photocatalysis; photoelectrochemistry water oxidation; water splitting
Categories
Funding
- Alliance for Molecular PhotoElectrode Design for Solar Fuels (AMPED), an Energy Frontier Research Center (EFRC) - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001011]
- National Science Foundation [ECCS-1542015]
- Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China [51888103]
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In this study, a semiconductor-mediator-catalyst structure was designed to fabricate an artificial photosynthesis electrode for water oxidation. The resulting hybrid assembly demonstrated enhanced photoelectrochemical water oxidation performance, attributed to the accelerated interfacial hole transfer and improved effective surface area.
In fabricating an artificial photosynthesis (AP) electrode for water oxidation, we have devised a semiconductor-mediator-catalyst structure that mimics photosystem II (PSII). It is based on a surface layer of vertically grown nanorods of Fe2O3 on fluorine doped tin oxide (FTO) electrodes with a carbazole mediator base and a Ru(II) carbene complex on a nanolayer of TiO2 as a water oxidation co-catalyst. The resulting hybrid assembly, FTO|Fe2O3|-carbazole|TiO2|-Ru(carbene), demonstrates an enhanced photoelectrochemical (PEC) water oxidation performance compared to an electrode without the added carbaozle base with an increase in photocurrent density of 2.2-fold at 0.95 V vs. NHE and a negatively shifted onset potential of 500 mV. The enhanced PEC performance is attributable to carbazole mediator accelerated interfacial hole transfer from Fe2O3 to the Ru(II) carbene co-catalyst, with an improved effective surface area for the water oxidation reaction and reduced charge transfer resistance.
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