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基于偏硼酸钠和过一硫酸盐的绿色催化氧化体系高效去除有机污染物。

Highly efficient removal of organic pollutants via a green catalytic oxidation system based on sodium metaborate and peroxymonosulfate.

机构信息

National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University, Hangzhou, 310018, PR China.

National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University, Hangzhou, 310018, PR China.

出版信息

Chemosphere. 2020 Jan;238:124687. doi: 10.1016/j.chemosphere.2019.124687. Epub 2019 Aug 27.

Abstract

The development of highly efficient and green catalytic oxidation process based on peroxymonosulfate (PMS) activation has been identified to be a significant yet challenging objective in the environmental catalysis field. A simple, environmentally benign and highly effective catalytic oxidation system was innovatively constructed by coupling NaBO and PMS for the removal of Acid Red 1. The catalytic mechanism in the NaBO/PMS system was elucidated by electron paramagnetic resonance (EPR) combined with several radical capture reagents (ascorbic acid, methanol, tert-butyl alcohol, ethanol and -histidine). The experimental results indicated that singlet oxygen (O) severed as the predominant reactive oxygen species (ROS) rather than the HO or during the catalytic oxidation process, at variance with the reported radical pathway in the Co/PMS system. Inspiringly, p-benzoquinone (p-BQ) as a trapping agent in most advanced oxidation process could be turned into the positive one in the NaBO/PMS system, achieving a nearly 3-times enhancement in terms of the rate constant for AR1 removal. More interestingly, sodium chloride (NaCl) presented the same enhancement effect as p-benzoquinone due to generation of hypochlorous acid (HOCl) and more O, which was completely different from the reported. This study develops a highly efficient green oxidation process and opens up a new insight in the remediation of contaminated water.

摘要

基于过一硫酸盐 (PMS) 活化的高效、绿色催化氧化方法的发展已被确定为环境催化领域的一个重要而具有挑战性的目标。本研究创新性地构建了一种简单、环境友好且高效的催化氧化体系,用于去除酸性红 1( Acid Red 1 )。通过电子顺磁共振(EPR)结合几种自由基捕获试剂(抗坏血酸、甲醇、叔丁醇、乙醇和 -组氨酸)对 NaBO/PMS 体系中的催化机制进行了阐明。实验结果表明,单线态氧(O )在催化氧化过程中作为主要的活性氧物种(ROS),而不是 HO 或 ,这与 Co/PMS 体系中报道的自由基途径不同。令人鼓舞的是,在大多数高级氧化过程中作为捕获剂的对苯醌(p-BQ)在 NaBO/PMS 体系中变为正电荷,对 AR1 去除的速率常数提高了近 3 倍。更有趣的是,由于次氯酸(HOCl)和更多 O 的产生,氯化钠(NaCl)表现出与对苯醌相同的增强效果,这与报道的完全不同。本研究开发了一种高效的绿色氧化方法,为受污染水的修复开辟了新的思路。

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