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photocatalytic co2 reduction highly enhanced by oxygen vacancies on Pt-nanoparticle-dispersed gallium oxide

Nano Research 2016年第6期9卷 1689-1700页

作者： Yun-Xiang Pan Zheng-Qing Sun Huai-Ping cong Yu-Long Men Sen Xin Jie Song Shu-Hong Yu School of Chemistry and Chemical Engineering Hefei University of Technology Hefei 230009 China Division ofNanomaterials & Chemistry Hefei National Laboratory for Physical Sciences at the Microscale Department of Chemistry CAS Center for Excellence in Nanoscience University of Science and Technology of China Hefei 230026 China Institute of Nano Biomedicine and Engineering Department of Instrument Science and Engineering School of Electronic Information and Electrical Engineering Shanghai Jiao Tong University Shanghai 200240 China

photocatalytic co2 reduction on metal-oxide-based catalysts is promising for solving the energy and environmental crises faced by mankind. The oxygen vacancy （Vo） on metal oxides is expected to be a key factor affecting the efficiency of photocatalytic co2 reduction on metal-oxide-based catalysts. Yet, to date, the question of how an Vo influences photocatalytic co2 reduction is still unanswered. Herein, we report that, on Vo-rich gallium oxide coated with Pt nanoparticles （Vo-rich Pt/Ga203）, co2 is photocatalytically reduced to co, with a highly enhanced co evolution rate （21.0umol.h-1） compared to those on Vo-poor Pt/Ga2O3 （3.9 gmol-h-1） and Pt/TiO2（P25）（6.7 gmol.h-1）. We demonstrate that the Vo leads to improved co2 adsorption and separation of the photoinduced charges on Pt/Ga203, thus enhancing the photocatalytic activity of Pt/Ga203. Rational fabrication of an Vo is thereby an attractive strategy for developing efficient catalysts for photocatalytic co2 reduction.

关键词： photocatalytic co2reduction oxygen vacancy metal-oxide-based catalyst C02 adsorption

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Enhanced CH4 yield by photocatalytic co2 reduction using TiO2 nanotube arrays grafted with Au, Ru, and ZnPd nanoparticles

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Nano Research 2016年第11期9卷 3478-3493页

作者： Piyush Kar Samira Farsinezhad Najia Mahdi Yun Zhang Uchenna Obuekwe Himani Sharma Jing Shen Natalia Semagina Karthik Shankar Department of Electrical and computer Engineering University of Alberta 9107-116 Street Edmonton Alberta T6G 2V4 Canada Department of Chemical & Materials Engineering University of Alberta 9107-116 Street Edmonton Alberta T66 2V4 Canada NRC National Institute for Nanotechnology 11421 Saskatchewan Dr. NW Edmonton Alberta T6G 2M9 Canada

Metal nanoparticle （NP） co-catalysts on metal oxide semiconductor supports are attracting attention as photocatalysts for a variety of chemical reactions. Related efforts seek to make and use Pt-free catalysts. In this regard, we report here enhanced CH4 formation rates of 25 and 60 μmol·g^-1·h^-1 by photocatalytic co2 reduction using hitherto unused ZnPd NPs as well as Au and Ru NPs. The NPs are formed by colloidal synthesis and grafted onto short n-type anatase TiO2 nanotube arrays （TNAs）, grown anodically on transparent glass substrates. The interfacial electric fields in the NP-grafted TiO2 nanotubes were probed by ultraviolet photoelectron spectroscopy （UPS）. Au NP-grafted TiO2 nanotubes （Au-TNAs） showed no band bending, but a depletion region was detected in Ru NP-grafted TNAs （Ru-TNAs） and an accumulation layer was observed in ZnPd NP-grafted TNAs （ZnPd-TNAs）. Temperature programmed desorption （TPD） experiments showed significantly greater co2 adsorption on NP-grafted TNAs. TNAs with grafted NPs exhibit broader and more intense UV-visible absorption bands than bare TNAs. We found that co2 photoreduction by nanoparticle-grafted TNAs was driven not only by ultraviolet photons with energies greater than the TiO2 band gap, but also by blue photons close to and below the anatase band edge. The enhanced rate of co2 reduction is attributed to superior use of blue photons in the solar spectrum, excellent reactant adsorption, efficient charge transfer to adsorbates, and low recombination losses.

关键词： metal nanoparticles (NPs) TiO2 nanotube arrays(TNAs) colloidal synthesis band bending built-in potential photocatalytic co2reduction semiconductorheterojunctions

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