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使用过氧乙酸的芬顿型工艺:效率、反应解析及生态毒性

Fenton-type process using peracetic acid: Efficiency, reaction elucidations and ecotoxicity.

作者信息

Carlos Thayrine Dias, Bezerra Leydiane Barbosa, Vieira Mayane Marques, Sarmento Renato Almeida, Pereira Douglas Henrique, Cavallini Grasiele Soares

机构信息

Programa de Pós-Graduação em Química, Universidade Federal do Tocantins, 77.402-970 Gurupi, Tocantins, Brazil.

Curso de Química Ambiental, Universidade Federal do Tocantins, 77.402-970 Gurupi, Tocantins, Brazil.

出版信息

J Hazard Mater. 2021 Feb 5;403:123949. doi: 10.1016/j.jhazmat.2020.123949. Epub 2020 Sep 15.

Abstract

Recent studies on Fenton-type processes involving peracetic acid (PAA) stimulated further development of advanced oxidative processes (AOPs). The objective of this work was to provide new information about such processes, elucidate their reaction mechanisms both experimentally and theoretically, and verify their possible uses. The Fenton-type reaction of PAA with Fe exhibited a greater dye degradation efficiency than the Fenton process, while the efficiency of the PAA reaction with Fe was very close of Fenton process. Moreover, the processes photocatalyzed by solar radiation demonstrated comparable efficiencies due to the photoreduction of Fe to Fe. By conducting theoretical calculations, it was found that the formation of oxidizing radicals during the reaction of PAA with Fe was not thermodynamically favorable and, therefore, unsuitable for practical use. In contrast, the processes occurred in the PAA/Fe system included thermodynamically spontaneous reactions that generated peroxyl (CHC(O)OO•), alkoxyl (CHC(O)•), and hydroperoxyl (HO•) radicals. The ecotoxicological tests demonstrated that the toxicity of the PAA to the organism Dugesia tigrina can be attributed to the presence of HO.

摘要

近期关于涉及过氧乙酸(PAA)的芬顿型过程的研究推动了高级氧化过程(AOPs)的进一步发展。这项工作的目的是提供有关此类过程的新信息,从实验和理论上阐明其反应机制,并验证其可能的用途。PAA与铁的芬顿型反应比芬顿过程表现出更高的染料降解效率,而PAA与铁反应的效率与芬顿过程非常接近。此外,由于铁被光还原为亚铁,太阳能辐射光催化的过程显示出相当的效率。通过进行理论计算,发现PAA与铁反应过程中氧化自由基的形成在热力学上不利,因此不适合实际应用。相比之下,PAA/铁体系中发生的过程包括产生过氧自由基(CHC(O)OO•)、烷氧自由基(CHC(O)•)和氢过氧自由基(HO•)的热力学自发反应。生态毒理学测试表明,PAA对生物三角涡虫的毒性可归因于HO的存在。

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