Surface-modified TiO<sub>2</sub> photocatalysts prepared by a photosynthetic route: Mechanism, enhancement, and limits (2024)

Abstract

Surface-modified TiO2 photocatalysts were synthesized by a photosynthetic route involving visible-light-induced (l> 455 nm) activation of benzene and toluene at the surface of TiO2 leading to the formation of carbonaceous polymeric deposits. IR spectroscopic and photoelectrochemical experiments showed that the mechanism of the photosynthetic reactions involves intra-bandgap surface states at TiO2 related to surface OH groups interacting with adsorbed aromatic molecules. The photosynthesized surface-modified TiO2 materials exhibited enhanced activity, relative to pristine TiO2, in photocatalytic degradation (and complete mineralization) of 4-chlorophenol. The improvement was pronounced particularly under visible-light (l>455 nm) irradiation with the relative initial photodegradation rate enhanced by a factor of four. The surface-modified photocatalysts exhibited good stability under the operating conditions, and the optimum carbon content was approximately 0.5 wt%. Mechanistic studies showed that the enhanced visible-light photodegradation of 4-chlorophenol is due to modified surface-adsorption properties that facilitate formation of a surface complex between titania and 4-chlorophenol, rather than due to any sensitizing effect of the carbonaceous deposits. The study highlights the importance of considering the interaction between pollutant molecules and the photocatalyst surface in heterogeneous photocatalysis, and possibly opens up a route for photosynthesis of further surface- modified photocatalysts with tuned surface properties.

Original languageEnglish
Pages (from-to)163-170
Number of pages8
JournalChemPlusChem
Volume79
Issue number1
DOIs
StatePublished - Jan 2014
Externally publishedYes

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Neubert, S., Ramakrishnan, A., Strunk, J., Shi, H., Mei, B., Wang, L., Bledowski, M., A. Guschin, D., Kauer, M., Wang, Y., Muhler, M., & Beranek, R. (2014). Surface-modified TiO2 photocatalysts prepared by a photosynthetic route: Mechanism, enhancement, and limits. ChemPlusChem, 79(1), 163-170. https://doi.org/10.1002/cplu.201300277

Neubert, Susann ; Ramakrishnan, Ayyappan ; Strunk, Jennifer et al. / Surface-modified TiO2 photocatalysts prepared by a photosynthetic route : Mechanism, enhancement, and limits. In: ChemPlusChem. 2014 ; Vol. 79, No. 1. pp. 163-170.

@article{f522a266ac37454b896e98ef22158aa6,

title = "Surface-modified TiO2 photocatalysts prepared by a photosynthetic route: Mechanism, enhancement, and limits",

abstract = "Surface-modified TiO2 photocatalysts were synthesized by a photosynthetic route involving visible-light-induced (l> 455 nm) activation of benzene and toluene at the surface of TiO2 leading to the formation of carbonaceous polymeric deposits. IR spectroscopic and photoelectrochemical experiments showed that the mechanism of the photosynthetic reactions involves intra-bandgap surface states at TiO2 related to surface OH groups interacting with adsorbed aromatic molecules. The photosynthesized surface-modified TiO2 materials exhibited enhanced activity, relative to pristine TiO2, in photocatalytic degradation (and complete mineralization) of 4-chlorophenol. The improvement was pronounced particularly under visible-light (l>455 nm) irradiation with the relative initial photodegradation rate enhanced by a factor of four. The surface-modified photocatalysts exhibited good stability under the operating conditions, and the optimum carbon content was approximately 0.5 wt%. Mechanistic studies showed that the enhanced visible-light photodegradation of 4-chlorophenol is due to modified surface-adsorption properties that facilitate formation of a surface complex between titania and 4-chlorophenol, rather than due to any sensitizing effect of the carbonaceous deposits. The study highlights the importance of considering the interaction between pollutant molecules and the photocatalyst surface in heterogeneous photocatalysis, and possibly opens up a route for photosynthesis of further surface- modified photocatalysts with tuned surface properties.",

author = "Susann Neubert and Ayyappan Ramakrishnan and Jennifer Strunk and Haoyu Shi and Bastian Mei and Lidong Wang and Michal Bledowski and {A. Guschin}, Dmitrii and Max Kauer and Yuemin Wang and Martin Muhler and Radim Beranek",

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doi = "10.1002/cplu.201300277",

language = "English",

volume = "79",

pages = "163--170",

journal = "ChemPlusChem",

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Neubert, S, Ramakrishnan, A, Strunk, J, Shi, H, Mei, B, Wang, L, Bledowski, M, A. Guschin, D, Kauer, M, Wang, Y, Muhler, M & Beranek, R 2014, 'Surface-modified TiO2 photocatalysts prepared by a photosynthetic route: Mechanism, enhancement, and limits', ChemPlusChem, vol. 79, no. 1, pp. 163-170. https://doi.org/10.1002/cplu.201300277

Surface-modified TiO2 photocatalysts prepared by a photosynthetic route: Mechanism, enhancement, and limits. / Neubert, Susann; Ramakrishnan, Ayyappan; Strunk, Jennifer et al.
In: ChemPlusChem, Vol. 79, No. 1, 01.2014, p. 163-170.

Research output: Contribution to journalArticlepeer-review

TY - JOUR

T1 - Surface-modified TiO2 photocatalysts prepared by a photosynthetic route

T2 - Mechanism, enhancement, and limits

AU - Neubert, Susann

AU - Ramakrishnan, Ayyappan

AU - Strunk, Jennifer

AU - Shi, Haoyu

AU - Mei, Bastian

AU - Wang, Lidong

AU - Bledowski, Michal

AU - A. Guschin, Dmitrii

AU - Kauer, Max

AU - Wang, Yuemin

AU - Muhler, Martin

AU - Beranek, Radim

PY - 2014/1

Y1 - 2014/1

N2 - Surface-modified TiO2 photocatalysts were synthesized by a photosynthetic route involving visible-light-induced (l> 455 nm) activation of benzene and toluene at the surface of TiO2 leading to the formation of carbonaceous polymeric deposits. IR spectroscopic and photoelectrochemical experiments showed that the mechanism of the photosynthetic reactions involves intra-bandgap surface states at TiO2 related to surface OH groups interacting with adsorbed aromatic molecules. The photosynthesized surface-modified TiO2 materials exhibited enhanced activity, relative to pristine TiO2, in photocatalytic degradation (and complete mineralization) of 4-chlorophenol. The improvement was pronounced particularly under visible-light (l>455 nm) irradiation with the relative initial photodegradation rate enhanced by a factor of four. The surface-modified photocatalysts exhibited good stability under the operating conditions, and the optimum carbon content was approximately 0.5 wt%. Mechanistic studies showed that the enhanced visible-light photodegradation of 4-chlorophenol is due to modified surface-adsorption properties that facilitate formation of a surface complex between titania and 4-chlorophenol, rather than due to any sensitizing effect of the carbonaceous deposits. The study highlights the importance of considering the interaction between pollutant molecules and the photocatalyst surface in heterogeneous photocatalysis, and possibly opens up a route for photosynthesis of further surface- modified photocatalysts with tuned surface properties.

AB - Surface-modified TiO2 photocatalysts were synthesized by a photosynthetic route involving visible-light-induced (l> 455 nm) activation of benzene and toluene at the surface of TiO2 leading to the formation of carbonaceous polymeric deposits. IR spectroscopic and photoelectrochemical experiments showed that the mechanism of the photosynthetic reactions involves intra-bandgap surface states at TiO2 related to surface OH groups interacting with adsorbed aromatic molecules. The photosynthesized surface-modified TiO2 materials exhibited enhanced activity, relative to pristine TiO2, in photocatalytic degradation (and complete mineralization) of 4-chlorophenol. The improvement was pronounced particularly under visible-light (l>455 nm) irradiation with the relative initial photodegradation rate enhanced by a factor of four. The surface-modified photocatalysts exhibited good stability under the operating conditions, and the optimum carbon content was approximately 0.5 wt%. Mechanistic studies showed that the enhanced visible-light photodegradation of 4-chlorophenol is due to modified surface-adsorption properties that facilitate formation of a surface complex between titania and 4-chlorophenol, rather than due to any sensitizing effect of the carbonaceous deposits. The study highlights the importance of considering the interaction between pollutant molecules and the photocatalyst surface in heterogeneous photocatalysis, and possibly opens up a route for photosynthesis of further surface- modified photocatalysts with tuned surface properties.

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Neubert S, Ramakrishnan A, Strunk J, Shi H, Mei B, Wang L et al. Surface-modified TiO2 photocatalysts prepared by a photosynthetic route: Mechanism, enhancement, and limits. ChemPlusChem. 2014 Jan;79(1):163-170. doi: 10.1002/cplu.201300277

Surface-modified TiO<sub>2</sub> photocatalysts prepared by a photosynthetic route: Mechanism, enhancement, and limits (2024)
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