Optimisation of degradation conditions of 1,8-diazabicyclo[5.4.0]undec-7-ene in water and reaction kinetics analysis using a cocurrent downflow contactor photocatalytic reactor

被引:51
|
作者
Ochuma, Idoko J. [1 ]
Fishwick, Robert P. [1 ]
Wood, Joseph [1 ]
Winterbottom, J. Mike [1 ]
机构
[1] Univ Birmingham, Dept Chem Engn, Birmingham B15 2TT, W Midlands, England
关键词
cocurrent downflow contactor; optimisation; photocatalysis; environment; kinetics;
D O I
10.1016/j.apcatb.2006.12.008
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
The photocatalytic degradation of 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU, a non-biodegradable nitrogenous organic compound) in water was optimised under UV radiation using titanium dioxide photocatalyst. The reactor used was a pilot scale cocurrent downflow contactor photocatalytic reactor (CDCPR), a system offering very high mass transfer efficiency. The effect of photocatalyst loading, initial substrate concentration, temperature, pH, and different combinations of UV, O-2, H2O2 and TiO2 on the photocatalytic oxidation of DBU was investigated. The TiO2 photocatalyst used was Degussa VPAeroperl P25/20, a granulated form of Degussa P-25, recently developed to ameliorate downstream catalyst separation problems. The CDCPR was fitted with an internally and vertically mounted 1.0 kW UV lamp. The reactions were carried out at 40-60 degrees C and 1 barg, with the reactor being operated in closed loop recycle mode and suspended photocatalyst being re-circulated. Optimisation of reaction conditions using a combination of TiO2, UV radiation and 02 gave the most rapid degradation and mineralisation of the DBU in comparison with other processes. Under optimised conditions, 100% degradation of DBU was achieved in 45 min, with a quantum yield of 7.39, using a 1 kW lamp, 0.5 g/dm(3) TiO2, 100 mg/dm(3) DBU, 1 barg, 50 degrees C and pH of 3.17. Investigating the reaction pathway and its modelling showed a first order dependency, incorporating the effect of first intermediates of degradation. The activation energy was found to be 54.68 kJ mol(-1) showing a significant influence of temperature on the photocatalytic degradation of DBU. (c) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:259 / 268
页数:10
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