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漆酶-介体系统对阿替洛尔的转化:效率、水成分的影响及转化途径。

Transformation of atenolol by a laccase-mediator system: Efficiencies, effect of water constituents, and transformation pathways.

机构信息

Guangzhou Key Laboratory 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, 510006, China.

Guangzhou Key Laboratory 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, 510006, China.

出版信息

Ecotoxicol Environ Saf. 2019 Nov 15;183:109555. doi: 10.1016/j.ecoenv.2019.109555. Epub 2019 Aug 13.

Abstract

In this study, we investigated the transformation of atenolol (ATL) by the naturally occurring laccase from Trametes versicolor in aqueous solution. Removal efficiency of ATL via laccase-catalyzed reaction in the presence of various laccase mediators was examined, and found that only the mediator 2, 2, 6, 6-tetramethyl-1-piperidinyloxy (TEMPO) was able to greatly promote ATL transformation. The influences of TEMPO concentration, laccase dosage, as well as solution pH and temperature on ATL transformation efficiency were tested. As TEMPO concentrations was increased from 0 to 2000 μM, ATL transformation efficiency first increased and then decreased, and the optimal TEMPO concentration was determined as 500 μM. ATL transformation efficiency was gradually increased with increasing laccase dosage. ATL transformation was highly pH-dependent with an optimum pH of 7.0, and it was almost constant over a temperature range of 25-50 °C. Humic acid inhibited ATL transformation through competition reaction with laccase. The presence of anions HCO and CO reduced ATL transformation due to both anions enhanced solution pHs, while Cl, SO, and NO at 10 mM showed no obvious influence. The main transformation products were identified, and the potential transformation pathways were proposed. After enzymatic treatment, the toxicity of ATL and TEMPO mixtures was greatly reduced. The results of this study might present an alternative clean strategy for the remediation of ATL contaminated water matrix.

摘要

在这项研究中,我们研究了漆酶(Trametes versicolor)自然产生的漆酶在水溶液中对阿替洛尔(ATL)的转化。考察了在各种漆酶介体存在下,通过漆酶催化反应去除 ATL 的效率,发现只有介体 2,2,6,6-四甲基-1-哌啶氧基(TEMPO)能够极大地促进 ATL 转化。测试了 TEMPO 浓度、漆酶用量以及溶液 pH 值和温度对 ATL 转化效率的影响。随着 TEMPO 浓度从 0 增加到 2000μM,ATL 转化效率先增加后降低,最佳 TEMPO 浓度确定为 500μM。ATL 转化效率随漆酶用量的增加而逐渐增加。ATL 转化对 pH 值高度依赖,最佳 pH 值为 7.0,在 25-50°C 的温度范围内几乎保持不变。腐殖酸通过与漆酶的竞争反应抑制 ATL 转化。阴离子 HCO 和 CO 的存在由于两种阴离子均增强了溶液 pH 值,从而降低了 ATL 转化,而 Cl、SO 和 NO 在 10mM 时则没有明显影响。鉴定了主要的转化产物,并提出了潜在的转化途径。酶处理后,ATL 和 TEMPO 混合物的毒性大大降低。本研究结果可能为 ATL 污染水基质的修复提供一种替代的清洁策略。

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