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过硫酸盐基高级氧化:机遇与障碍的批判性评估。

Persulfate-Based Advanced Oxidation: Critical Assessment of Opportunities and Roadblocks.

机构信息

School of Civil, Environmental, and Architectural Engineering, Korea University, Seoul 136-701, Korea.

Eawag, Swiss Federal Institute of Aquatic Science and Technology, Überlandstrasse 133, CH-8600, Düebendorf, Switzerland.

出版信息

Environ Sci Technol. 2020 Mar 17;54(6):3064-3081. doi: 10.1021/acs.est.9b07082. Epub 2020 Feb 27.

DOI:10.1021/acs.est.9b07082
PMID:32062964
Abstract

Reports that promote persulfate-based advanced oxidation process (AOP) as a viable alternative to hydrogen peroxide-based processes have been rapidly accumulating in recent water treatment literature. Various strategies to activate peroxide bonds in persulfate precursors have been proposed and the capacity to degrade a wide range of organic pollutants has been demonstrated. Compared to traditional AOPs in which hydroxyl radical serves as the main oxidant, persulfate-based AOPs have been claimed to involve different in situ generated oxidants such as sulfate radical and singlet oxygen as well as nonradical oxidation pathways. However, there exist controversial observations and interpretations around some of these claims, challenging robust scientific progress of this technology toward practical use. This Critical Review comparatively examines the activation mechanisms of peroxymonosulfate and peroxydisulfate and the formation pathways of oxidizing species. Properties of the main oxidizing species are scrutinized and the role of singlet oxygen is debated. In addition, the impacts of water parameters and constituents such as pH, background organic matter, halide, phosphate, and carbonate on persulfate-driven chemistry are discussed. The opportunity for niche applications is also presented, emphasizing the need for parallel efforts to remove currently prevalent knowledge roadblocks.

摘要

近年来,有关过硫酸盐基高级氧化工艺(AOP)作为替代基于过氧化氢工艺的可行性的报告在水处理文献中迅速增加。已经提出了各种激活过硫酸盐前体中过氧键的策略,并证明了其降解各种有机污染物的能力。与以羟基自由基为主要氧化剂的传统 AOP 相比,过硫酸盐基 AOP 据称涉及不同的原位生成氧化剂,如硫酸根自由基和单线态氧以及非自由基氧化途径。然而,围绕其中一些说法存在有争议的观察和解释,这对该技术向实际应用的稳健科学进展构成了挑战。本综述批判性地比较了过一硫酸盐和过二硫酸盐的活化机制以及氧化物种的形成途径。主要氧化物种的性质受到仔细审查, singlet oxygen 的作用存在争议。此外,还讨论了水参数和成分(如 pH 值、背景有机物、卤素、磷酸盐和碳酸盐)对过硫酸盐驱动化学的影响。还介绍了利基应用的机会,强调需要共同努力消除当前普遍存在的知识障碍。

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