Influence of relative humidity on the photocatalytic oxidation (PCO) of toluene by TiO2 loaded on activated carbon fibers:: PCO rate and intermediates accumulation

被引:158
作者
Guo, Ting [1 ]
Bai, Zhipeng [1 ]
Wu, Can [1 ]
Zhu, Tan [1 ]
机构
[1] Nankai Univ, Coll Environm Sci & Engn, State Environm Protect Key Lab Urban Ambient Air, Tianjin 300071, Peoples R China
关键词
photocatalytic oxidation; intermediates; relative humidity (RH); TiO2/ACF; toluene;
D O I
10.1016/j.apcatb.2007.09.033
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 [物理化学]; 081704 [应用化学];
摘要
Photocatalytic oxidation (PCO) tests were carried out for toluene adsorbed on the activated carbon fibers (ACFs)-supported TiO2 photocatalyst in an environmental condition controlled chamber. TiO2/ACF catalyst was made and characterized by N-2 adsorption isotherm for pore structure and scanning electron microscopy (SEM) for morphology, respectively. Through exploring the remnant of toluene and the accumulation of intermediates on the TiO2/ACF catalyst including species, amount and their change processes under different relative humidity (RH), this study aimed to explore the influence of RH on the PCO of toluene and the roles of water vapor in the PCO process: PCO reaction paths and the accumulation of intermediates on the TiO2/ACF catalyst. Results showed that (1) with the increase of RH in the chamber (15%, 30%, 45% and 60%) the PCO conversion rate of toluene was positive correlated and no catalyst deactivation was observed under all RH levels; (2) during the gas-solid PCO process of toluene, byproducts of aromatic ring oxidation including 2-methyl, p-benzoquinone and o(m, p)-cresol were observed on the Ti02/ACF catalyst which had not been reported, together with the intermediates of side chain oxidation including benzyl alcohol, benzaldehyde and benzoic acid which had been reported; (3) although benzaldehyde was the primary intermediate under all RH level, amounts of the byproducts of aromatic ring oxidation were increased with the increase of RH; and (4) elevated RH increased the accumulation of benzyl alcohol but assuredly decreased the accumulation of benzaldehyde. These results suggested that (1) RH affects both the PCO rate and the PCO reaction path of toluene; (2) although methyl group oxidation is the major path, aromatic ring oxidation, which is not the expected path for the PCO of toluene, is enhanced when the RH increases; (3) apart from the role of hydroxyl radical ((OH)-O-center dot) produced from water by TiO2, water molecule also directly takes part in the PCO process. A hypothesis has been suggested: transition species comprised of benzaldehyde, hydroxyl and water molecule exists in the PCO conversion process from benzaldehyde to benzoic acid, though the hypothesis has not been confirmed. (c) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:171 / 178
页数:8
相关论文
共 28 条
[1]
Reversible catalyst deactivation in the photocatalytic oxidation of dilute o-xylene in air [J].
Ameen, MM ;
Raupp, GB .
JOURNAL OF CATALYSIS, 1999, 184 (01) :112-122
[2]
Combination effect of activated carbon with TiO2 for the photodegradation of binary pollutants at typical indoor air level [J].
Ao, CH ;
Lee, SC .
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY, 2004, 161 (2-3) :131-140
[3]
Enhancement effect of TiO2 immobilized on activated carbon filter for the photodegradation of pollutants at typical indoor air level [J].
Ao, CH ;
Lee, SC .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2003, 44 (03) :191-205
[4]
TiO2 activation by using activated carbon as a support -: Part II.: Photoreactivity and FTIR study [J].
Araña, J ;
Doña-Rodríguez, JM ;
Rendón, ET ;
Cabo, CGI ;
González-Díaz, O ;
Herrera-Melián, JA ;
Pérez-Peña, J ;
Colón, G ;
Navío, JA .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2003, 44 (02) :153-160
[5]
TiO2 activation by using activated carbon as a support -: Part I.: Surface characterisation and decantability study [J].
Araña, J ;
Doña-Rodríguez, JM ;
Rendón, ET ;
Cabo, CGI ;
González-Díaz, O ;
Herrera-Melián, JA ;
Pérez-Peña, J ;
Colón, G ;
Navío, JA .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2003, 44 (02) :161-172
[6]
BERMAN E, 1993, P 3 INT S CHEM OX TE
[7]
SELECTIVITY CONTROL DURING THE PHOTOASSISTED OXIDATION OF 1-BUTANOL ON TITANIUM-DIOXIDE [J].
BLAKE, NR ;
GRIFFIN, GL .
JOURNAL OF PHYSICAL CHEMISTRY, 1988, 92 (20) :5697-5701
[8]
Photocatalytic oxidation of toluene on nanoscale TiO2 catalysts:: Studies of deactivation and regeneration [J].
Cao, LX ;
Gao, Z ;
Suib, SL ;
Obee, TN ;
Hay, SO ;
Freihaut, JD .
JOURNAL OF CATALYSIS, 2000, 196 (02) :253-261
[9]
Benzene and toluene gas-phase photocatalytic degradation over H2O and HCL pretreated TiO2:: by-products and mechanisms [J].
d'Hennezel, O ;
Pichat, P ;
Ollis, DF .
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY, 1998, 118 (03) :197-204
[10]
FLUIDIZED-BED PHOTOCATALYTIC OXIDATION OF TRICHLOROETHYLENE IN CONTAMINATED AIRSTREAMS [J].
DIBBLE, LA ;
RAUPP, GB .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1992, 26 (03) :492-495