On the Kinetics and Mechanism of Electrochemical Decomposition of 3-Chloropyridine in Aqueous Solution

被引:4
作者
Ma, Xiangjuan [1 ]
Ding, Jingfeng [1 ]
Bian, Lixia [1 ]
Zhou, Minghua [2 ]
机构
[1] Zhejiang Gongshang Univ, Sch Environm Sci & Engn, Hangzhou 310012, Zhejiang, Peoples R China
[2] Nankai Univ, Coll Environm Sci & Engn, Minist Educ, Key Lab Pollut Proc & Environm Criteria, Tianjin 300071, Peoples R China
基金
中国国家自然科学基金;
关键词
Electrochemical decomposition; Kinetics; mechanism; 3-chloropyridine; WASTE-WATER TREATMENT; LEAD DIOXIDE; ACTIVATED CARBON; PYRIDINES; DEGRADATION; ADSORPTION; OXIDATION; POLLUTANTS; ELECTRODE; ABATEMENT;
D O I
10.2174/138527212803251668
中图分类号
O62 [有机化学];
学科分类号
070303 ; 081704 ;
摘要
Electrochemical oxidation of 3-chloropyridine (3-ClPYR), as a model pollutant, on a modified beta-PbO2 electrode was examined by bulk electrolysis. Parameters affecting the removal and reaction rate of 3-ClPYR, such as current density, pH and initial concentration, were investigated. The results showed that 3-ClPYR could be readily decomposed under the attack of hydroxyl radicals (OH) electrochemically generated on the modified beta-PbO2 anode, the removal of 3-ClPYR was confirmed satisfactorily to fit pseudo-first order kinetics, the rate constant was mainly governed by current density and pH of 3-ClPYR solution. The evolution of intermediates was examined with 200 mg.L-1 of 3-ClPYR at pH 6.2, 3.0 g. L-1 of Na2SO4 and 160 mA cm(-2) of current density. Pyridine was firstly formed via starting with the scission of C-Cl bond. When the initial concentration of 3-ClPYR was above 600 mg.L-1, 2, 3-dichloropyridine and 3, 5-dichloropyridine were also detected in a very small quantities owing to the addition of chlorine radicals (Cl). Then, pyridine and chlorinated pyridine were further cleaved to organic acids (oxalic acid, acetic acid, formic acid and propionic acid) and inorganic ions (Cl-, NO2-, NO3-, ClO-) via opening the nitrogen containing heterocyclic ring, indicating the promising use of electrochemical technique for clean and safe removal of nitrogen containing heterocyclic compounds from industrial effluents.
引用
收藏
页码:1972 / 1977
页数:6
相关论文
共 26 条
[1]   Biodegradation of pyridine using aerobic granules in the presence of phenol [J].
Adav, Sunil S. ;
Lee, Duu-Jong ;
Ren, N. Q. .
WATER RESEARCH, 2007, 41 (13) :2903-2910
[2]   ROLE OF PYRIDINE N-OXIDE IN THE CYTOTOXICITY AND GENOTOXICITY OF CHLOROPYRIDINES [J].
ANUSZEWSKA, EL ;
KOZIOROWSKA, JH .
TOXICOLOGY IN VITRO, 1995, 9 (02) :91-94
[3]   Photocatalytic degradation of chlorinated pyridines in titania aqueous suspensions [J].
Aramendia, M. A. ;
Colmenares, J. C. ;
Lopez-Fernandez, S. ;
Marinas, A. ;
Marinas, J. M. ;
Moreno, J. M. ;
Urbano, F. J. .
CATALYSIS TODAY, 2008, 138 (1-2) :110-116
[4]   Mapping the photocatalytic activity or potential free radical toxicity of nanoscale titania [J].
Barnard, Amanda S. .
ENERGY & ENVIRONMENTAL SCIENCE, 2011, 4 (02) :439-443
[5]   High-performance Ti/BDD electrodes for pollutant oxidation [J].
Chen, XM ;
Chen, GH ;
Gao, FR ;
Yue, PL .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2003, 37 (21) :5021-5026
[6]   COMPARATIVE MUTAGENICITY OF HALOGENATED PYRIDINES IN THE SALMONELLA-TYPHIMURIUM MAMMALIAN MICROSOME TEST [J].
CLAXTON, LD ;
DEARFIELD, KL ;
SPANGGORD, RJ ;
RICCIO, ES ;
MORTELMANS, K .
MUTATION RESEARCH, 1987, 176 (02) :185-198
[7]   Electrocatalytic generation of radical intermediates over lead dioxide electrode doped with fluoride [J].
Cong, Yanqing ;
Wu, Zucheng .
JOURNAL OF PHYSICAL CHEMISTRY C, 2007, 111 (08) :3442-3446
[8]   Direct Reduction of Nitrite to N2 on a Pt(100) Electrode in Alkaline Media [J].
Duca, Matteo ;
Cucarella, Mar Oroval ;
Rodriguez, Paramaconi ;
Koper, Marc T. M. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (51) :18042-18044
[9]   Electrochemical oxidation of organic pollutants for the wastewater treatment: direct and indirect processes [J].
Martinez-Huitle, Carlos A. ;
Ferro, Sergio .
CHEMICAL SOCIETY REVIEWS, 2006, 35 (12) :1324-1340
[10]   Kinetic Study of the Electrochemical Oxidation of Salicylic Acid and Salicylaldehyde Using UV/vis Spectroscopy and Multivariate Calibration [J].
Matyasovszky, Nelson ;
Tian, Min ;
Chen, Aicheng .
JOURNAL OF PHYSICAL CHEMISTRY A, 2009, 113 (33) :9348-9353