Online Quantification of O2·- and H2O2 and Their Formation Kinetics in Ultraviolet (UV)-Irradiated Nano-TiO2 Suspensions by Continuous Flow Chemiluminescence

doi:10.6023/A15010036

Acta Chim. Sinica ›› 2015, Vol. 73 ›› Issue (5): 388-394.DOI: 10.6023/A15010036 Previous Articles Next Articles

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连续流动化学发光法在线定量检测二氧化钛光催化产生的O₂^·-和H₂O₂及其生成动力学研究

王大彬, 赵利霞, 郭良宏, 张辉, 万斌, 杨郁

中国科学院生态环境研究中心环境化学与生态毒理学国家重点实验室 100085

投稿日期:2015-01-14 发布日期:2015-03-20
通讯作者: 赵利霞 E-mail:zlx@rcees.ac.cn,lhguo@rcees.ac.cn
基金资助:
项目受国家重点基础研究计划(No. 2011CB936001)和国家自然科学基金(Nos. 21177138, 21207146, 21477146, 21377142)资助.

Online Quantification of O₂^·- and H₂O₂ and Their Formation Kinetics in Ultraviolet (UV)-Irradiated Nano-TiO₂ Suspensions by Continuous Flow Chemiluminescence

Wang Dabin, Zhao Lixia, Guo Lianghong, Zhang Hui, Wan Bin, Yang Yu

State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085

Received:2015-01-14 Published:2015-03-20
Supported by:
Project supported by the National Basic Research Program of China (No. 2011CB936001) and the National Natural Science Foundation of China (Nos. 21177138, 21207146, 21477146, 21377142).

O₂^·- and H₂O₂, the two reactive oxygen species (ROS) produced in TiO₂ photocatalytic reactions, play important roles in the photodegradation of pollutants. In this work, according to the different lifetime of O₂^·- and H₂O₂, online quantification of O₂^·- and H₂O₂ was successfully achieved based on the two established continuous flow chemiluminescence (CFCL) methods using luminol as the chemiluminescence probe. For O₂^·-, the CL intensity was detected by mixing the irradiated TiO₂ suspension containing O₂^·- with luminol within 10 s due to its short lifetime and poor stability, and thus the concentration of O₂^·- was indirectly quantified according to the linear relationship between the CL intensity and the luminol concentration. For H₂O₂ detection with the luminol/K₃Fe(CN)₆ system, the CL intensity was detected after the irradiated TiO₂ suspension was placed in darkness for 30 min to ensure the complete disappearance of O₂^·-, and the concentration of H₂O₂ produced was directly quantified by the calibration curve between the CL intensity and H₂O₂ concentration. The concentration of O₂^·- and H₂O₂ was determined approximately in the range of 7.5～30 nmol/L and 0.60～3.0 μmol/L, and the detection limit was 1.95 nmol/L and 18.0 nmol/L respectively. Based on the proposed models of O₂^·- and H₂O₂ formation, the kinetic process of O₂^·- and H₂O₂ formation was studied, and both of them followed the increase of exponential decay function. By simulating the time-dependent concentration change of O₂^·- and H₂O₂ with their kinetic formulas, the formation rate constants (k_f) of O₂^·- and H₂O₂ were calculated to be 0.0653 nmol·s^-1, and 15.0 nmol·s^-1 respectively. The formation rate of H₂O₂ was higher than that of O₂^·- in the TiO₂ photocatalytic reactions. This work provides us more insight into the formation process of ROS, and may help to improve the photocatalytic efficiency of TiO₂ photocatalysis.

Key words: continuous flow chemiluminescence, TiO₂ photocatalysis, O₂^·-, H₂O₂, on-line quantification, kinetic study

Cite this article

Wang Dabin, Zhao Lixia, Guo Lianghong, Zhang Hui, Wan Bin, Yang Yu. Online Quantification of O₂^·- and H₂O₂ and Their Formation Kinetics in Ultraviolet (UV)-Irradiated Nano-TiO₂ Suspensions by Continuous Flow Chemiluminescence[J]. Acta Chim. Sinica, 2015, 73(5): 388-394.

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连续流动化学发光法在线定量检测二氧化钛光催化产生的O₂^·-和H₂O₂及其生成动力学研究

Online Quantification of O₂^·- and H₂O₂ and Their Formation Kinetics in Ultraviolet (UV)-Irradiated Nano-TiO₂ Suspensions by Continuous Flow Chemiluminescence

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连续流动化学发光法在线定量检测二氧化钛光催化产生的O2·-和H2O2及其生成动力学研究