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固定化漆酶于中空介孔碳纳米球:显著的固定化效果、优异的稳定性和高效去除抗生素污染物的能力。

Immobilization of laccase on hollow mesoporous carbon nanospheres: Noteworthy immobilization, excellent stability and efficacious for antibiotic contaminants removal.

机构信息

College of Environmental Science and Engineering, Hunan University and Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China.

College of Environmental Science and Engineering, Hunan University and Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China.

出版信息

J Hazard Mater. 2019 Jan 15;362:318-326. doi: 10.1016/j.jhazmat.2018.08.069. Epub 2018 Sep 14.

DOI:10.1016/j.jhazmat.2018.08.069
PMID:30243255
Abstract

In this study, the hollow mesoporous carbon spheres (HMCs) were synthesized and modified for laccase (Lac) immobilization, and the structural characteristics of HMCs materials were determined by FESEM, TEM and FTIR etc. The maximum loading of Lac on the HMCs materials could reach 835 mg/g, meanwhile, the immobilized Lac exhibited excellent thermo-stability, pH stability, storage stability and reusability. The antibiotics removal experiments indicated that the immobilized Lac possess efficient removal efficiency for both tetracycline hydrochloride (TCH) and ciprofloxacin hydrochloride (CPH) in the presence of redox mediator. The synergy of the adsorption by HMCs and the degradation by Lac could be the reasons for the high removal of antibiotics. Meanwhile, for investigating degradation mechanism, the degradation product analysis and molecular docking method had been introduced to this study. According to the degradation products, dehydroxylation and demethylation are major degradation reactions for TCH degradation, and the oxidation of the piperazinyl substituent and hydroxylation are the major degradation for CPH degradation. The docking results showed that some important residues played the key role in the degradation process. This study indicated that the immobilization of Lac on HMCs could be potentially applied in environmental remediation of antibiotics.

摘要

在这项研究中,合成了中空介孔碳球(HMCs)并对其进行了修饰以固定漆酶(Lac),通过 FESEM、TEM 和 FTIR 等方法确定了 HMCs 材料的结构特征。HMCs 材料对 Lac 的最大负载量可达 835mg/g,同时,固定化 Lac 表现出优异的热稳定性、pH 稳定性、储存稳定性和可重复使用性。抗生素去除实验表明,在氧化还原介体存在的情况下,固定化 Lac 对盐酸四环素(TCH)和盐酸环丙沙星(CPH)均具有高效的去除效率。HMCs 的吸附和 Lac 的降解之间的协同作用可能是抗生素去除效率高的原因。同时,为了研究降解机制,本研究引入了降解产物分析和分子对接方法。根据降解产物,TCH 降解的主要反应是去羟化和去甲基化,而 CPH 降解的主要反应是哌嗪取代基的氧化和羟基化。对接结果表明,一些重要的残基在降解过程中发挥了关键作用。本研究表明,Lac 固定化在 HMCs 上可能在抗生素的环境修复中具有潜在的应用价值。

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