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顺序可见光驱动光催化和漆酶催化降解五氯酚和 2,4-二氯酚。

Degradation of pentachlorophenol and 2,4-dichlorophenol by sequential visible-light driven photocatalysis and laccase catalysis.

机构信息

State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, Beijing 100875, PR China.

出版信息

Environ Sci Technol. 2010 Dec 1;44(23):9117-22. doi: 10.1021/es1025432. Epub 2010 Nov 4.

Abstract

Chlorophenols (CPs) can be degraded by visible-light driven photocatalysis or laccase catalysis. However, previous and present studies have shown that neither of the two methods was efficient when being used individually. Low degradation rates were observed for the degradation of pentachlorophenol (PCP) by laccase-catalysis and that of 2,4-dichlorophenol (2,4-DCP) by photocatalysis. To remove CPs more completely, a sequential photolaccase catalytic system was designed to degrade PCP and 2,4-DCP mixture in water at the optimal pH value. The results showed that photocatalysis prior to laccase-catalysis (PPL) is a better approach than laccase-catalysis prior to photocatalysis (LPP), eliminating CPs more efficiently and generating lower toxic products. The identified intermediate products consisted of adipic acid, hexanediol, glycol, propylene glycol, hydroquinol, and phthalandione. Based on the products identified, the sequential degradation process was proposed, including the interlace reactions involving quinoid oxidation, reductive dechlorination, and no-enzyme polymerization. Upon reaction optimization, a piston flow reactor (PFR) was designed to treat the continuous feeding of simulated wastewater containing PCP and 2,4-DCP. After a 128 h period of treatment, 87.4-99.5% total concentration of CPs were removed (PPL removed 99.7% PCP and 99.2% 2,4-DCP; LPP removed 95.9% PCP and 78.9% 2,4-DCP).

摘要

氯酚(CPs)可通过可见光驱动的光催化或漆酶催化进行降解。然而,以前和现在的研究表明,这两种方法单独使用时都效率不高。酶催化降解五氯酚(PCP)和光催化降解 2,4-二氯酚(2,4-DCP)的降解速率都较低。为了更彻底地去除 CPs,设计了一个顺序光漆酶催化系统,在最佳 pH 值下在水中降解 PCP 和 2,4-DCP 混合物。结果表明,光催化先于漆酶催化(PPL)比漆酶催化先于光催化(LPP)更好,更有效地去除 CPs,并生成更少的有毒产物。鉴定出的中间产物包括己二酸、己二醇、乙二醇、丙二醇、氢醌和邻苯二甲二酮。根据鉴定出的产物,提出了顺序降解过程,包括涉及醌氧化、还原脱氯和无酶聚合的交错反应。在反应优化后,设计了活塞流反应器(PFR)来处理含有 PCP 和 2,4-DCP 的模拟废水的连续进料。经过 128 h 的处理,CPs 的总浓度去除率达到 87.4-99.5%(PPL 去除了 99.7%的 PCP 和 99.2%的 2,4-DCP;LPP 去除了 95.9%的 PCP 和 78.9%的 2,4-DCP)。

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