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Abstract
Enhancement of visible-light photocurrent generation by sol–gel anatase TiO2 films was achieved by binding small polyol molecules to the TiO2 surface. Binding ethylene glycol onto the surface, enhancement factors up to 2.8 were found in visible-light photocurrent generation experiments. Density functional theory calculations identified midgap energy states that emerge as a result of the binding of a range of polyols to the TiO2 surface. The presence and energy of the midgap state is predicted to depend sensitively on the structure of the polyol, correlating well with the photocurrent generation results. Together, these results suggest a new, facile, and cost-effective route to precise surface band gap engineering of TiO2 toward visible-light-induced photocatalysis and energy storage.
Highlights
An increasing number of important processes are being transitioned to using sunlight as their energy source,[1,2] including pollutant degradation,[3−7] photocurrent generation,[8−11] and high energy content chemical synthesis.[12−16] In designing devices for these applications, a fine balance must be struck between the energy-conversion efficiency of the device, the lifetime of the end product, and other factors, such as material cost/abundance, toxicity, and physicochemical stability.[17]
Much effort has been expended to elementary idnocpreinasge,22th−e25visdibylee-lisgehntsiatciztiavtiitoyno,2f6T−2iO8 2,pilnacsmludoinnigc enhancement,[15,29] and surface modification by organic molecules.[30−32] visible-light activity was achieved in these approaches, sacrifices were made in terms of material performance
The effect of the molecular adsorption on the photoactivity of sol−gel derived anatase TiO2 films on fluorine tin oxide (FTO) in visible light was found in photocurrent generation experiments, an analysis tool successfully employed in similar studies on semiconductor photoactivity.[34,35]
Summary
An increasing number of important processes are being transitioned to using sunlight as their energy source,[1,2] including pollutant degradation,[3−7] photocurrent generation,[8−11] and high energy content chemical synthesis.[12−16] In designing devices for these applications, a fine balance must be struck between the energy-conversion efficiency of the device, the lifetime of the end product, and other factors, such as material cost/abundance, toxicity, and physicochemical stability.[17]. One of the biggest drawbacks in the TiO2 applications is its wide band gap (∼3.2 eV for the most active crystal form, anatase TiO2) This limits the spectral range of absorbable solar photons to the UV region (λ < 400 nm); only about 5% of the light reaches the earth’s surface.[17,21] Much effort has been expended to elementary idnocpreinasge,22th−e25visdibylee-lisgehntsiatciztiavtiitoyno,2f6T−2iO8 2,pilnacsmludoinnigc enhancement,[15,29] and surface modification by organic molecules.[30−32] visible-light activity was achieved in these approaches, sacrifices were made in terms of material performance. The energy of these mid-band-gap states is found to depend on the polyol structure, allowing surface DOS engineering and optimization of TiO2 visible photoactivity in a facile and cost-effective manner
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