School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China; School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, GA 30332, USA.
School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China.
Water Res. 2021 Feb 1;189:116605. doi: 10.1016/j.watres.2020.116605. Epub 2020 Nov 4.
With the fast development of peroxymonosulfate (PMS)-dominating processes in drinking water and wastewater treatment, residual PMS is easy to come across chlorine as these processes are usually followed by secondary chlorine disinfection. The synergistic effect of PMS and chlorine on the degradation of micro-organic pollutants is investigated by selecting acetaminophen (ACT) as a reference compound for the first time in this study. Unlike conventional PMS or chlorine activation which generates reactive species such as hydroxyl radical (HO), sulfate radical (SO), chlorine radical (Cl), and singlet oxygen (O), the efficient ACT removal is attributed to the direct catalytic chlorination by PMS due to the significantly enhanced consumption of chlorine along with negligible change of PMS concentration at neutral condition, and the same reaction pathways in both PMS/chlorine and chlorine processes. The kinetic study demonstrates that ACT oxidation by PMS/chlorine follows second order reaction, and the degradation efficiency can be promoted at alkaline conditions with peak rate constants at pH 9.0-10.0. The presence of chloride can enhance the removal of ACT, while ammonium and humic acid significantly retard ACT degradation. Higher formation of selected disinfection by-products (DBPs) is observed in the PMS/chlorine process than in the sole chlorination. This study highlights the important role of PMS in organic pollutants degradation and DBPs formation during the chlorination process.
随着过一硫酸盐(PMS)主导的饮用水和废水处理工艺的快速发展,由于这些工艺通常紧随二次氯消毒,因此很容易遇到残留的 PMS。本研究首次选择对乙酰氨基酚(ACT)作为参考化合物,研究了 PMS 和氯对降解微量有机污染物的协同作用。与传统的 PMS 或氯活化不同,后者会产生活性物质,如羟基自由基(HO)、硫酸根自由基(SO)、氯自由基(Cl)和单线态氧(O),而在中性条件下,由于 PMS 浓度的显著变化,ACT 的有效去除归因于 PMS 的直接催化氯化,同时氯的消耗明显增加,在 PMS/氯和氯工艺中均具有相同的反应途径。动力学研究表明,PMS/氯对 ACT 的氧化遵循二级反应,在碱性条件下可以促进降解效率,在 pH9.0-10.0 时有峰值速率常数。氯离子的存在可以提高 ACT 的去除率,而铵和腐殖酸则会显著减缓 ACT 的降解。在 PMS/氯工艺中观察到的选定消毒副产物(DBP)的形成量高于单独氯化。本研究强调了 PMS 在氯化过程中对有机污染物降解和 DBP 形成的重要作用。