Journal article
Engineering titania nanostructure to tune and improve its photocatalytic activity
Proceedings of the National Academy of Sciences - PNAS, v 113(15), pp 3966-3971
12 Apr 2016
PMID: 27035977
Featured in Collection : UN Sustainable Development Goals @ Drexel
Abstract
This work shows that hole−electron recombination can be controlled by engineering the length of brookite nanorods, and that a variety of organic substrates can be efficiently oxidized as the counterreaction to hydrogen evolution. Both are important steps to developing photocatalysis as a sustainable technology. Electron−hole recombination is a major fundamental limitation in any photocatalytic process. By controlling and reducing it with rod length, we can increase the efficiency of photocatalyzed processes. Also, by utilizing demanding substrates in aqueous media, ethanol, glucose, and glycerol, we make a step toward the photoreforming of more plentiful feedstocks such as, or derived from, biomass.
Photocatalytic pathways could prove crucial to the sustainable production of fuels and chemicals required for a carbon-neutral society. Electron−hole recombination is a critical problem that has, so far, limited the efficiency of the most promising photocatalytic materials. Here, we show the efficacy of anisotropy in improving charge separation and thereby boosting the activity of a titania (TiO
2
) photocatalytic system. Specifically, we show that H
2
production in uniform, one-dimensional brookite titania nanorods is highly enhanced by engineering their length. By using complimentary characterization techniques to separately probe excited electrons and holes, we link the high observed reaction rates to the anisotropic structure, which favors efficient carrier utilization. Quantum yield values for hydrogen production from ethanol, glycerol, and glucose as high as 65%, 35%, and 6%, respectively, demonstrate the promise and generality of this approach for improving the photoactivity of semiconducting nanostructures for a wide range of reacting systems.
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Details
- Title
- Engineering titania nanostructure to tune and improve its photocatalytic activity
- Creators
- Matteo Cargnello - Department of ChemistryTiziano Montini - Department of Chemical and Pharmaceutical Sciences, Institute of Chemistry of Organometallic Compounds, National Research Council (CNR), National Interuniversity Consortium of Materials Science and Technology (INSTM)Sergey Y Smolin - Department of Chemical and Biological EngineeringJacqueline B Priebe - Leibniz-Institut für Katalyse e.VJuan J Delgado Jaén - Departamento de Ciencia de los Materiales e Ingeniería Metalúrgica y Química Inorgánica, Facultad de CienciasVicky V. T Doan-Nguyen - Department of Materials Science and EngineeringIan S McKay - Department of Chemical EngineeringJay A Schwalbe - Department of Chemical EngineeringMarga-Martina Pohl - Leibniz-Institut für Katalyse e.VThomas R Gordon - Department of ChemistryYupeng Lu - Department of Materials Science and EngineeringJason B Baxter - Department of Chemical and Biological EngineeringAngelika Brückner - Leibniz-Institut für Katalyse e.VPaolo Fornasiero - Department of Chemical and Pharmaceutical Sciences, Institute of Chemistry of Organometallic Compounds, National Research Council (CNR), National Interuniversity Consortium of Materials Science and Technology (INSTM)Christopher B Murray - Department of Chemistry
- Publication Details
- Proceedings of the National Academy of Sciences - PNAS, v 113(15), pp 3966-3971
- Publisher
- National Academy of Sciences
- Grant note
- ECCS-1201957 / National Science Foundation (NSF) CBET-1335821 / National Science Foundation (NSF) CBET-1333649 / National Science Foundation (NSF)
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Chemical and Biological Engineering
- Web of Science ID
- WOS:000373762400034
- Scopus ID
- 2-s2.0-84963538015
- Other Identifier
- 991014877704904721
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- Collaboration types
- Domestic collaboration
- International collaboration
- Web of Science research areas
- Chemistry, Physical