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过氧乙酸-三价铁体系中投加吡啶甲酸强化去除水中微量污染物。

Enhanced Degradation of Micropollutants in a Peracetic Acid-Fe(III) System with Picolinic Acid.

机构信息

School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States.

Department of Chemistry and Biochemistry, Spelman College, Atlanta, Georgia 30314, United States.

出版信息

Environ Sci Technol. 2022 Apr 5;56(7):4437-4446. doi: 10.1021/acs.est.1c08311. Epub 2022 Mar 23.

Abstract

Activation of peracetic acid (PAA) with iron species is an emerging advanced oxidation process (AOP). This study investigates the use of the chelating agent picolinic acid (PICA) to extend the pH range and enhance the performance of the PAA-Fe(III) AOP. Compared to the PAA-Fe(III) system, the PAA-Fe(III)-PICA system degrades various micropollutants (MPs: methylene blue, naproxen, sulfamethoxazole, carbamazepine, trimethoprim, diclofenac, and bisphenol-A) much more rapidly at higher pH, achieving almost complete removal of parent compounds within 10 min. PAA significantly outperforms the coexistent HO and is the key oxidant for rapid compound degradation. Other chelating agents, EDTA, NTA, citric acid, proline, and nicotinic acid, could not enhance MP degradation in the PAA-Fe(III) system, while 2,6-pyridinedicarboxylic acid with a structure similar to PICA moderately enhanced MP degradation. Experiments with scavengers (-butyl alcohol and methyl phenyl sulfoxide) and a probe compound (benzoic acid) confirmed that high-valent iron species [Fe(IV) and/or Fe(V)], rather than radicals, are the major reactive species contributing to MP degradation. The oxidation products of methylene blue, naproxen, and sulfamethoxazole by PAA-Fe(III)-PICA were characterized and supported the proposed mechanism. This work demonstrates that PICA is an effective complexing ligand to assist the Fenton reaction of PAA by extending the applicable pH range and accelerating the catalytic ability of Fe(III).

摘要

过氧乙酸 (PAA) 与铁物种的活化是一种新兴的高级氧化工艺 (AOP)。本研究考察了螯合剂吡啶甲酸 (PICA) 的使用,以扩展 pH 范围并提高 PAA-Fe(III) AOP 的性能。与 PAA-Fe(III) 系统相比,PAA-Fe(III)-PICA 系统在较高 pH 值下更快地降解各种微量污染物 (MPs:亚甲蓝、萘普生、磺胺甲恶唑、卡马西平、甲氧苄啶、双氯芬酸和双酚 A),在 10 分钟内几乎完全去除母体化合物。PAA 明显优于共存的 HO,是快速化合物降解的关键氧化剂。其他螯合剂,如 EDTA、NTA、柠檬酸、脯氨酸和烟酸,不能增强 PAA-Fe(III) 系统中 MPs 的降解,而结构类似于 PICA 的 2,6-吡啶二甲酸则适度增强了 MPs 的降解。使用清除剂(-丁醇和甲基苯基亚砜)和探针化合物(苯甲酸)的实验证实,高价铁物种 [Fe(IV) 和/或 Fe(V)],而不是自由基,是导致 MPs 降解的主要反应性物质。通过 PAA-Fe(III)-PICA 氧化产物的特征分析,支持了所提出的反应机制。这项工作表明,PICA 是一种有效的络合剂,可以通过扩展适用的 pH 范围和加速 Fe(III)的催化能力来辅助 PAA 的芬顿反应。

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