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可见光无催化剂活化过硫酸盐用于水消毒:效率和机制。

Catalyst-free activation of persulfate by visible light for water disinfection: Efficiency and mechanisms.

机构信息

Guangzhou Key Laboratory of Environmental Catalysis and Pollution Control, Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, School of Environmental Science and Engineering, Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou, China.

Guangzhou Key Laboratory of Environmental Catalysis and Pollution Control, Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, School of Environmental Science and Engineering, Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou, China.

出版信息

Water Res. 2019 Jun 15;157:106-118. doi: 10.1016/j.watres.2019.03.071. Epub 2019 Mar 28.

Abstract

The development of cost-effective water disinfection methods is highly desired to address the problems caused by outbreak of harmful microorganisms. Sulfate radical (•SO)-based advanced oxidation technology has attracted increasing attention. However, various catalysts or UV irradiation are usually used to activate persulfate (PS), which is high-cost and the recovery of nano-sized catalysts is also challenging. This work demonstrates a new method of catalyst-free activation of persulfate by visible light (VL) for bacterial inactivation. The 6-log of E. coli cells can be inactivated within 40 min and 7-log of E. coli cells could be inactivated within 120 min by the VL/PS system. The major responsive wavelength is 420 nm, and no heat activation of PS is found during VL irradiation. A synergistic effect with synergy factor of 51.2% is found when combining the VL irradiation with heating at 50 °C. The acidic pH is benefit for the VL/PS-triggered bacterial inactivation, while bicarbonate inhibits the E. coli inactivation at the range of 0.1-20 mg/L. Mechanism study indicates the main reactive species are •SO, •O and •OH, in which •SO plays the most important role. The bacterial inactivation process shows to begin from outer membrane to intracellular components. Subsequently, the antioxidant enzyme (i.e. SOD, CAT) is induced, followed by damaging to the genomic DNA leading to fatal death of the cells. In addition, the VL/PS system is also applicable for the inactivation of other pathogenic bacteria, including Staphylococcus aureus and Pseudomonas aeruginosa, showing universality for water disinfection applications. This work not only provides a new cost-effective disinfection method without a catalyst, but also sheds light on understanding the bacterial inactivation mechanism by •SO-based AOPs.

摘要

为了解决有害微生物爆发所带来的问题,人们强烈希望开发具有成本效益的水消毒方法。基于硫酸根自由基(•SO )的高级氧化技术受到了越来越多的关注。然而,通常使用各种催化剂或紫外线(UV)辐照来激活过硫酸盐(PS),这既昂贵又难以回收纳米级催化剂。本工作展示了一种通过可见光(VL)无催化剂激活过硫酸盐用于细菌灭活的新方法。在 40 min 内可以灭活 6 对数的大肠杆菌细胞,在 120 min 内可以灭活 7 对数的大肠杆菌细胞。主要响应波长为 420nm,并且在 VL 辐照期间未发现 PS 的热激活。当将 VL 辐照与 50°C 的加热相结合时,发现协同作用的协同因子为 51.2%。酸性 pH 有利于 VL/PS 引发的细菌灭活,而碳酸氢盐在 0.1-20mg/L 的范围内抑制大肠杆菌的灭活。机理研究表明,主要的活性物质是•SO、•O 和•OH,其中•SO 起最重要的作用。细菌灭活过程从外膜开始到细胞内成分。随后,诱导抗氧化酶(即 SOD、CAT),接着破坏基因组 DNA,导致细胞致命死亡。此外,VL/PS 系统也适用于其他致病菌(包括金黄色葡萄球菌和铜绿假单胞菌)的灭活,表明其在水消毒应用中的通用性。这项工作不仅提供了一种新的、具有成本效益的无催化剂消毒方法,而且还阐明了基于•SO 的 AOPs 对细菌灭活机制的认识。

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