Chloride ion activate peroxymonosulfate for degradation of trimethoprim in aqueous solution

doi:10.16085/j.issn.1000-6613.2017-1528

Abstract

Abstract: In this work,the kinetics and mechanisms of TMP degradation by chloride ion (Cl^-) directly reacting with peroxymonosulfate (PMS)were investigate by selecting typical pharmaceuticals and personal care products (PPCP)of trimethoprim (TMP)as target compounds. The effect of degradation efficiency was compared between chlorination and Cl^-/PMS. Some factors affecting degradation was investigated,such as ammonium ions (NH⁴⁺),nitrate ions (NO^3-),carbonate ions (CO₃^2-),bicarbonate ions (HCO₃^-),temperature and humic acid. The results showed that TMP degradation fitted well with the pseudo-first-order kinetics. The pseudo-first-order-constant (k_obs)is 0.0296min^-1 (R²>0.97). kobs decreased with the increase of initial TMP concentration. The degradation efficiency of TMP by chlorination and Cl^-/PMS was similar,but the reaction rate of Cl^-/PMS was slower than that of chlorination. The presence of NH⁴⁺ will inhibit the degradation,and chlorination is more sensitive to NH⁴⁺. CO₃^2- and HCO₃^- are harmful to the degradation of TMP,and the greater concentration of CO₃^2-,the stronger inhibition effect,the greater the concentration of HCO₃^-,the weaker inhibition effect. Increasing solution temperature will efficiently accelerate the degradation of TMP. The reaction activation energy is 66.97kJ/mol. The presence of humic acid also retarded the removal of TMP to a certain extent.

Key words: trimethoprim, peroxymonosulfate, active chlorine, reaction kinetics

摘要： 以水中典型药物及个人护理品甲氧苄啶（TMP）为目标污染物，研究了氯离子活化过一硫酸钾（PMS）氧化降解TMP的效能和机理；对比了氯氧化工艺和Cl^-活化PMS对TMP的去除效能；考察了底物初始浓度、NH⁴⁺、NO^3-、CO₃^2-、HCO₃^-、温度和腐植酸对TMP降解的影响。研究表明，TMP降解过程符合拟一级反应动力学模型，反应动力学常数为0.0296min^-1（R² >0.97）；随着TMP初始浓度的增加，反应速率常数kobs减小；氯氧化工艺和Cl^-活化PMS对TMP的去除率相近，但Cl^-活化PMS降解TMP的反应速率较慢。NH⁴⁺的存在会抑制降解反应，并且氯氧化工艺对NH⁴⁺更敏感；NO^3-对降解反应无影响；CO₃^2-和HCO₃^-的会抑制降解反应，CO₃^2-浓度越大，抑制作用越强。HCO₃^-浓度越大，抑制作用越弱；温度越高，反应速率常数越大。根据阿伦尼乌斯方程，得到TMP的反应活化能Ea为66.97kJ/mol；溶液中腐植酸浓度越大，TMP的去除率越小。

关键词: 过一硫酸钾, 甲氧苄啶, 活性氯, 反应动力学

CLC Number:

GU Zhenchuan, GAO Naiyun, AN Na, CHEN Juxiang. Chloride ion activate peroxymonosulfate for degradation of trimethoprim in aqueous solution[J]. Chemical Industry and Engineering Progress, 2018, 37(05): 1992-1998.

古振川, 高乃云, 安娜, 陈菊香. 氯离子活化过一硫酸钾降解水中甲氧苄啶[J]. 化工进展, 2018, 37(05): 1992-1998.

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