Electrocatalytic generation of radical intermediates over lead dioxide electrode doped with fluoride

被引:90
作者
Cong, Yanqing [1 ]
Wu, Zucheng [1 ]
机构
[1] Zhejiang Univ, Dept Environm Engn, Hangzhou 310027, Peoples R China
关键词
D O I
10.1021/jp066362w
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
Electrochemical processes have provided promising contributions for environmental protection. A novel lead dioxide electrode doped with fluoride was investigated for wastewater treatment. The modified beta-PbO2, electrode showed high chemical stability and catalytic activity for contaminants abatement and organic mineralization. Evidence for active free radicals generation in electrochemical degradation was shown by electron spin resonance spectroscopy (ESR). 5,5-Dimethyl-1-pyrroline-N-oxide (DMPO) was used as spin trapping agent. The characteristic of hydroxyl radicals, 5,5-dimethyl-2-hydroxypyrrilidine-N-oxyI (DMPO-OH) spin adduct, was observed and the additions of hydroxyl radical scavengers reduce the signal of DMPO-OH. This indicated that hydroxyl radicals were indeed formed and played a critical role in water treatment. 4-Chlorophenol was chosen as model pollutant and the prepared electrode exhibited the perfect catalytic activity. The origin of the electrode and the structure of the anodic layer were examined to understand the mechanism of hydroxyl radical formation. The electrochemical reactions occurred at beta-PbO2 electrode was rather complex and involved the crystal-hydrated layer. It is the most environmentally friendly treatment method to use electrogenerated hydroxyl radicals as oxidants.
引用
收藏
页码:3442 / 3446
页数:5
相关论文
共 24 条
[1]  
Berger P, 2002, ENVIRON SCI TECHNOL, V36, P3083
[2]   ELECTROCATALYSIS IN THE ELECTROCHEMICAL CONVERSION/COMBUSTION OF ORGANIC POLLUTANTS FOR WASTE-WATER TREATMENT [J].
COMNINELLIS, C .
ELECTROCHIMICA ACTA, 1994, 39 (11-12) :1857-1862
[3]  
Cong Yan-qing, 2004, J Zhejiang Univ Sci, V5, P180, DOI 10.1631/jzus.2004.0180
[4]   Electrokinetic behaviour of chlorinated phenols in soil and their electrochemical degradation [J].
Cong, YQ ;
Ye, Q ;
Wu, ZC .
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION, 2005, 83 (B2) :178-183
[5]   ELECTROCATALYTIC PROCESSES ON PB/PBO2 ELECTRODES AT HIGH ANODIC POTENTIAL [J].
DANILOV, FI ;
VELICHENKO, AB ;
NISHCHERYAKOVA, LN .
ELECTROCHIMICA ACTA, 1994, 39 (11-12) :1603-1605
[6]   Electrochemical oxidation of 4-chlorophenol for wastewater treatment -: Definition of normalized current efficiency (φ) [J].
Gherardini, L ;
Michaud, PA ;
Panizza, M ;
Comninellis, C ;
Vatistas, N .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2001, 148 (06) :D78-D82
[7]   Electrocatalysis of anodic oxygen-transfer reactions: Bi3Ru3O11 electrodes in acidic media [J].
He, L ;
Anderson, JR ;
Franzen, HF ;
Johnson, DC .
CHEMISTRY OF MATERIALS, 1997, 9 (03) :715-722
[8]   Determination of hydroxyl radicals in an advanced oxidation process with salicylic acid trapping and liquid chromatography [J].
Jen, JF ;
Leu, MF ;
Yang, TC .
JOURNAL OF CHROMATOGRAPHY A, 1998, 796 (02) :283-288
[9]   Electrochemical incineration of 4-chlorophenol and the identification of products and intermediates by mass spectrometry [J].
Johnson, SK ;
Houk, LL ;
Feng, JR ;
Houk, RS ;
Johnson, DC .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1999, 33 (15) :2638-2644
[10]   Determination of the hydroxyl radical by its adduct formation with phenol and liquid chromatography/electrochemical detection [J].
Kilinc, E .
TALANTA, 2005, 65 (04) :876-881