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[1]王鹏莺,苏冰琴,彭娅娅,等.过一硫酸盐直接氧化降解吡啶的反应条件和机制[J].中国给水排水,2022,38(13):64-70.
　WANGPeng-ying,SUBing-qin,PENGYa-ya,et al.Reaction Conditions and Mechanism of Peroxymonosulfate for Direct Oxidative Degradation of Pyridine[J].China Water & Wastewater,2022,38(13):64-70.

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过一硫酸盐直接氧化降解吡啶的反应条件和机制

中国给水排水[ISSN:1000-4062/CN:12-1073/TU] 卷: 第38卷期数: 2022年第13期页码: 64-70 栏目: 出版日期: 2022-07-01

Title:: Reaction Conditions and Mechanism of Peroxymonosulfate for Direct Oxidative Degradation of Pyridine

作者:: 王鹏莺^1,2，苏冰琴^1,2，彭娅娅¹，温宇涛^1,2，郭越^1,2，李瑞¹; （1.太原理工大学环境科学与工程学院，山西太原 030024；2.山西省市政工程研究生教育创新中心，山西太原 030024）

Author(s):: WANG　Peng-ying^1，2， SU　Bing-qin^1，2， PENG　Ya-ya¹， WEN　Yu-tao^1，2， GUO　Yue^1，2， LI　Rui¹; （1. College of Environmental Science and Engineering， Taiyuan University of Technology， Taiyuan 030024， China； 2. Municipal Engineering Graduate Education Innovation Center of Shanxi Province， Taiyuan 030024， China）

关键词:: 过一硫酸盐; 直接氧化; 吡啶; 氮杂环化合物; 反应机制

Keywords:: peroxymonosulfate; direct oxidation; pyridine; nitrogen heterocyclic compound; reaction mechanism

摘要:: 采用过一硫酸盐（PMS）直接氧化降解废水中的氮杂环化合物吡啶，考察了PMS投加量、pH、共存阴离子（Cl^-、HCO₃^-、NO₃^-）和腐殖酸（HA）对吡啶降解效果的影响。结果表明，PMS直接氧化去除吡啶的过程符合拟一级反应动力学。当吡啶初始浓度为8.0 mg/L、pH为7.0、反应温度为25 ℃、PMS投加量为4.0 mmol/L时，反应150 min后对吡啶的降解率可达到93.66%。水中Cl^-、HCO₃^-、NO₃^-和HA的存在均对吡啶的降解没有明显影响。自由基鉴定实验结果显示，PMS体系中未产生硫酸根自由基（SO₄^-·）和羟基自由基（·OH），有少量单线态氧（¹O₂）生成，PMS的直接氧化作用是吡啶降解的主要因素。通过GC-MS分析检测到PMS直接氧化降解吡啶的中间产物为N，N-二甲基丙烯酰胺、草酸、乙酸等低毒性有机化合物。

Abstract:: Peroxymonosulfate (PMS) was directly applied to oxidize nitrogen heterocyclic compound pyridine in wastewater. The effects of PMS dosage, pH, coexisting anions（Cl^-, HCO₃^-, NO₃^-）and humic acid (HA) on degradation of pyridine were investigated. The direct oxidation of pyridine by PMS conformed to pseudo first-order reaction kinetics. When the initial concentration of pyridine was 8.0 mg/L, the pH was 7.0, the reaction temperature was 25 ℃, and PMS dosage was 4.0 mmol/L, the removal efficiency of pyridine reached 93.66% after 150 minutes of reaction. The presence of Cl^-, HCO₃^-, NO₃^- and HA in water had no significant effect on pyridine degradation. Free radical identification showed that no sulfate radical (SO₄^-·) and hydroxyl radical (·OH) were generated, and a small amount of singlet oxygen (¹O₂) was formed in the PMS system. The direct oxidation of PMS was the main mechanism of pyridine degradation. GC-MS analysis showed that the intermediate products of pyridine directly oxidized by PMS were N, N-dimethylacrylamide, oxalic acid, acetic acid, and other low?toxic organic compounds.

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更新日期/Last Update: 2022-07-01