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用电化学高级氧化工艺去除水中的莠去津及其副产物。

Removal of atrazine and its by-products from water using electrochemical advanced oxidation processes.

机构信息

Institut National de la Recherche Scientifique (INRS-Centre Eau, Terre et Environnement), Université du Québec, 490 rue de la Couronne, Québec, QC, G1K 9A9, Canada.

Institut de Chimie et Procédés pour l'Énergie, l'Environnement et la Santé (ICPEES), CNRS, Université de Strasbourg, rue Victor Demange, 57500, Saint-Avold, France.

出版信息

Water Res. 2017 Nov 15;125:91-103. doi: 10.1016/j.watres.2017.08.036. Epub 2017 Aug 17.

Abstract

Atrazine (ATZ) is one of the most common pesticides detected in surface water in Quebec (Canada). The present study was mainly focused on the degradation of ATZ and its by-products using electrochemical advanced oxidation processes such as photo-electro-Fenton (PEF), electro-Fenton (EF) and anodic-oxidation with simultaneous HO formation (AO - HO). The comparison of these processes showed that PEF process was found to be the most effective process in removing ATZ and its by-products from both synthetic solution (ATZ = 100 μg L) and real agricultural surface water enriched with ATZ (ATZ = 10 μg L). Different operating parameters, including wavelength of the light, pH, current density and the presence of natural organic matter (humic acids) were investigated for PEF process using boron-doped diamond (BDD) anode and graphite cathode. The current density and the wavelength of the light were the most important parameters in the ATZ degradation efficiency. The best operating conditions were recorded for the synthetic samples at a current density of 18.2 mA cm, a pH of 3.0 and treatment time of 45 min. Results showed that atrazine-desethyl-desisopropyl (DEDIA) was the most important by-product recorded. More than 99% of ATZ oxidation was recorded after 15 min of treatment and all the concentrations of major by-products were less than the limit of detection after 45 min of treatment. The PEF process was also tested for real surface water contaminated by ATZ: i) with and without addition of iron; ii) without pH adjustment (pH ∼ 6.7) and with pH adjustment (pH ∼ 3.1). In spite of the presence of radical scavenger and iron complexation the PEF process was more effective to remove ATZ from real surface water when the pH value was adjusted near to 3.0. The ATZ removal was 96.0% with 0.01 mM of iron (k = 0.13 min) and 100% with 0.1 mM of iron (k = 0.17 min).

摘要

莠去津(ATZ)是加拿大魁北克省地表水检测到的最常见的农药之一。本研究主要集中在使用电化学高级氧化工艺(如光电芬顿(PEF)、电芬顿(EF)和同时形成羟基自由基的阳极氧化(AO-HO))来降解莠去津及其副产物。这些过程的比较表明,PEF 过程被发现是从合成溶液(莠去津=100μg/L)和富含莠去津的实际农业地表水中去除莠去津及其副产物的最有效过程(莠去津=10μg/L)。使用掺硼金刚石(BDD)阳极和石墨阴极研究了不同的操作参数,包括光的波长、pH 值、电流密度和天然有机物(腐殖酸)的存在,对 PEF 过程进行了研究。电流密度和光的波长是 ATZ 降解效率的最重要参数。在电流密度为 18.2 mA/cm、pH 值为 3.0 和处理时间为 45 min 的情况下,记录到了最佳的操作条件。结果表明,记录到的最重要的副产物是莠去津去乙基去异丙基(DEDIA)。在处理 15 min 后,莠去津的氧化率超过 99%,在处理 45 min 后,所有主要副产物的浓度均低于检测限。PEF 工艺也用于被莠去津污染的实际地表水:i)有和没有添加铁;ii)不调节 pH 值(pH∼6.7)和调节 pH 值(pH∼3.1)。尽管存在自由基清除剂和铁络合物,但当 pH 值调节到接近 3.0 时,PEF 工艺更有效地从实际地表水去除莠去津。当铁浓度为 0.01 mM(k=0.13 min)和 0.1 mM(k=0.17 min)时,莠去津的去除率分别为 96.0%和 100%。

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