Competitive role of structural properties of titania-silica mixed oxides and a mechanistic study of the photocatalytic degradation of phenol

被引:38
作者
Rasalingam, Shivatharsiny [1 ]
Kibombo, Harrison S. [1 ]
Wu, Chia-Ming [1 ]
Peng, Rui [1 ]
Baltrusaitis, Jonas [2 ]
Koodali, Ranjit T. [1 ]
机构
[1] Univ S Dakota, Dept Chem, Vermillion, SD 57069 USA
[2] Univ Twente, PhotoCatalyt Synth Grp, NL-7500 AE Enschede, Netherlands
基金
美国国家科学基金会;
关键词
Photocatalysts; Titania-silica; Phenol; Heterolinkages; Crystallinity; ENHANCED PHOTOACTIVITY; MESOPOROUS SILICA; TIO2; PARTICLES; SUPPORTED TIO2; OXIDATION; WATER; 4-CHLOROPHENOL; TIO2/SIO2; PHOTODEGRADATION; DECOMPOSITION;
D O I
10.1016/j.apcatb.2013.11.025
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
TiO2-SiO2 mixed oxide materials were hydrothermally synthesized and the photocatalytic degradation of phenol under UV-irradiation was evaluated. We also demonstrated that varying the co-solvent, modulates the structural properties of the materials. In particular, the use of non-polar co-solvents such as toluene seemed to increase the crystallinity, surface area, and pore diameter while the crystallite size of titania seemed to change little. A comprehensive characterization using surface and bulk techniques evidenced the role of porosities, crystallinity, and Ti-O-Si linkages of the mixed oxides as significant factors that contribute to the degradation of phenol. The TiO2-SiO2 mixed oxide material prepared using only ethanol as the solvent showed 24% degradation of phenol after 120 mm of irradiation whereas other mixed oxide materials degraded phenol more efficiently (57% to 100%) in the same duration of time. The higher photocatalytic activities of the mixed oxide materials prepared using non-polar solvents is attributed to a combination of factors that include higher Apparent Surface Coverages of Ti-O-Si heterolinkages, larger pore sizes, and most importantly higher crystallinities of the titania phase. Larger pore sizes enabled better transport of reactant molecules and products to and from the active sites (Ti-O-Si heterolinkages) and the higher crystallinities of the titania phase helped in minimizing the electron-hole recombination in these photocatalysts, and thus resulted in high degradation efficiencies. (C) 2013 Elsevier B.V. All rights reserved.
引用
收藏
页码:394 / 405
页数:12
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