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A Semiconductor-Mediator-Catalyst Artificial Photosynthetic System for Photoelectrochemical Water Oxidation |
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| Authors: | Dr. Fujun Niu Dr. Degao Wang Dr. Lenzi J. Williams Dr. Animesh Nayak Prof. Fei Li Dr. Xiangyan Chen Dr. Ludovic Troian-Gautier Prof. Qing Huang Prof. Yanming Liu Dr. M. Kyle Brennaman Prof. John M. Papanikolas Prof. Liejin Guo Prof. Shaohua Shen Prof. Thomas J. Meyer |
| Affiliation: | 1. International Research Center for Renewable Energy (IRCRE) State Key Laboratory of Multiphase Flow in Power Engineering (MFPE), Xi'an Jiaotong University (XJTU), 28 West Xianning Road, Xi'an, Shaanxi, 710049 P. R. China Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina, 27599 United States These authors contributed equally to this work.;2. Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina, 27599 United States Engineering Laboratory of Advanced Energy Materials Ningbo Institute of Industrial Technology, Chinese Academy of Sciences, Ningbo, Zhejiang, 315201 P. R. China These authors contributed equally to this work.;3. Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina, 27599 United States;4. International Research Center for Renewable Energy (IRCRE) State Key Laboratory of Multiphase Flow in Power Engineering (MFPE), Xi'an Jiaotong University (XJTU), 28 West Xianning Road, Xi'an, Shaanxi, 710049 P. R. China;5. Engineering Laboratory of Advanced Energy Materials Ningbo Institute of Industrial Technology, Chinese Academy of Sciences, Ningbo, Zhejiang, 315201 P. R. China |
| Abstract: | 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. |
| Keywords: | heterogeneous catalysis photocatalysis photoelectrochemistry water oxidation water splitting |