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Minute Cu2+ coupling with HCO3− for efficient degradation of acetaminophen via H2O2 activation
Ecotoxicology and Environmental Safety ( IF 6.2 ) Pub Date : 2021-06-16 , DOI: 10.1016/j.ecoenv.2021.112422
Yimin Zhang 1 , Jingkun Lou 1 , Leliang Wu 1 , Minghua Nie 2 , Caixia Yan 1 , Mingjun Ding 1 , Peng Wang 1 , Hua Zhang 1
Affiliation  

Homogeneous Cu2+-mediated activation of H2O2 has been widely applied for the removal of organic contaminants, but fairly high dosage of Cu2+ is generally required and may cause secondary pollution. In the present study, minute Cu2+ (2.5 μM) catalyzed H2O2 exhibited excellent efficiency in degradation of organic pollutants with the assistant of naturally occurring level HCO3 (1 mM). In a typical case, acetaminophen (ACE) was completely eliminated within 10 min which followed the pseudo-first-order kinetics. Singlet oxygen and superoxide radical rather than traditionally identified hydroxyl radical were the predominant reactive oxygen species (ROS) responsible for ACE degradation. Meanwhile, Cu3+ was deduced through Cu+ and p-hydroxybenzoic acid formation analysis. CuCO3(aq) was the main complex with high reactivity for the activation of H2O2 to form ROS and Cu3+. The removal efficiency of ACE depended on the operating parameters, such as Cu2+, HCO3 and H2O2 dosage, solution initial pH. The presence of Cl, HPO42−, humic acid were found to retard ACE removal while other anions such as SO42− and NO3 had no obvious effect. ACE exhibited lower degradation efficiency in real water matrices than that in ultra-pure water. Nevertheless, 58–100% of ACE was removed from domestic wastewater, lake water and tap water within 60 min. Moreover, eight intermediate products were identified and the possible degradation pathways of ACE were proposed. Additionally, other typical organic pollutants including bisphenol A, norfloxacin, lomefloxacin hydrochloride and sulfadiazine, exhibited great removal efficiency in the Cu2+/H2O2/HCO3 system.



中文翻译:

分钟 Cu 2+与 HCO 3 偶联,通过 H 2 O 2活化有效降解对乙酰氨基酚

均相Cu 2+介导的H 2 O 2活化已广泛应用于有机污染物的去除,但通常需要相当高的Cu 2+剂量并且可能造成二次污染。在本研究中,微小的 Cu 2+ (2.5 μM) 催化的 H 2 O 2在天然存在的 HCO 3 -水平的辅助下,在降解有机污染物方面表现出优异的效率。(1 毫米)。在典型情况下,对乙酰氨基酚 (ACE) 在 10 分钟内完全消除,遵循伪一级动力学。单线态氧和超氧自由基而不是传统上确定的羟基自由基是导致 ACE 降解的主要活性氧 (ROS)。同时,通过Cu +羟基苯甲酸形成分析推导出Cu 3+。CuCO 3 (aq) 是主要的配合物,对于激活 H 2 O 2形成 ROS 和 Cu 3+具有高反应性。ACE的去除效率取决于操作参数,如Cu 2+、HCO 3 -和H2 O 2用量,溶液初始pH值。发现Cl -、HPO 4 2-、腐殖酸的存在会延缓ACE 的去除,而其他阴离子如SO 4 2-和NO 3 -没有明显影响。ACE 在实际水基质中的降解效率低于在超纯水中的降解效率。尽管如此,58-100% 的 ACE 在 60 分钟内从生活废水、湖水和自来水中去除。此外,还鉴定了 8 种中间产物,并提出了 ACE 可能的降解途径。此外,其他典型有机污染物包括双酚 A、诺氟沙星、盐酸洛美沙星和磺胺嘧啶,在 Cu 中表现出很好的去除效率。2+ /H 2 O 2 /HCO 3 -系统。

更新日期:2021-06-17
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