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Enhanced Degradation of Perfluorocarboxylic Acids (PFCAs) by UV/Sulfite Treatment: Reaction Mechanisms and System Efficiencies at pH 12
Environmental Science & Technology Letters ( IF 8.9 ) Pub Date : 2020-04-23 , DOI: 10.1021/acs.estlett.0c00236
Michael J. Bentel 1 , Zekun Liu 1 , Yaochun Yu 1, 2 , Jinyu Gao 1 , Yujie Men 1, 2 , Jinyong Liu 1
Affiliation  

Reductive defluorination with UV-generated hydrated electrons (eaq) is a promising technology for the destruction of perfluorocarboxylic acids (PFCAs, CnF2n+1COO). However, prior studies using pH 9–10 observed a slow reaction rate, limited defluorination percentage (deF%), and thus high energy consumption. Herein, we report on the substantially enhanced rate and extent of PFCA defluorination by operating the UV/sulfite system at the optimized pH 12. Degradation kinetics and transformation products show that at pH 12 the eaq cleaved multiple strong C–F bonds that could not be cleaved at pH 9.5. The high pH condition also significantly favored the preferred decarboxylation pathway toward a deep defluorination. In comparison to the reactions at pH 9.5, the increase in solution pH to 12 improved the UV lamp energy efficiency by 5–22 folds, enhanced the deF% of C3–C9 PFCAs to 73%–93%, and reduced the overall consumption of chemicals.

中文翻译:

UV /亚硫酸盐处理增强的全氟羧酸(PFCA)降解:pH值为12时的反应机理和系统效率

还原脱氟用UV生成水合电子(ë水溶液- )是用于全氟羧酸的破坏(全氟羧酸,C有前途的技术Ñ ˚F 2 Ñ 1 COO - )。但是,先前使用pH 9-10进行的研究发现反应速度慢,脱氟百分率(deF%)有限,因此能耗高。在此,我们通过在优化的pH 12.降解动力学操作所述UV /亚硫酸盐系统上的显着增强PFCA脱氟的速率和程度报告,并转化产物表明,在pH值为12的ë水溶液-断裂了多个在pH 9.5时无法断裂的强CF键。高pH条件也显着促进了优选的脱羧途径,从而实现了深度脱氟。与pH 9.5时的反应相比,溶液pH值增加到12可将紫外线灯的能量效率提高5-22倍,将C3-C9 PFCA的deF%提高到73%-93%,并减少化学药品。
更新日期:2020-04-23
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