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一种用于从水、废水和湖水中去除多环芳烃和药物及个人护理产品的可持续漆酶@M-多壁碳纳米管纳米杂化系统。

A sustainable nano-hybrid system of laccase@M-MWCNTs for multifunctional PAHs and PhACs removal from water, wastewater, and lake water.

作者信息

Grmasha Ruqayah Ali, Al-Sareji Osamah J, Meiczinger Mónika, Stenger-Kovács Csilla, Al-Juboori Raed A, Jakab Miklós, Lengyel Edina, Somogyi Viola, Khan Mohammad Amir, Hashim Khalid S

机构信息

Sustainability Solutions Research Lab, Faculty of Engineering, University of Pannonia, Egyetem str. 10, Veszprém H, 8200, Hungary; Environmental Research and Studies Center, University of Babylon, Babylon, Al-Hillah,51001, Iraq; University of Pannonia, Faculty of Engineering, Center for Natural Science, Research Group of Limnology, H-8200, Veszprem, Egyetem u. 10, Hungary; The School of Civil and Environmental Engineering graduate, University of New South Wales, Sydney, Kensington, NSW, 2052, Australia.

Sustainability Solutions Research Lab, Faculty of Engineering, University of Pannonia, Egyetem str. 10, Veszprém H, 8200, Hungary; Environmental Research and Studies Center, University of Babylon, Babylon, Al-Hillah,51001, Iraq; The School of Civil and Environmental Engineering graduate, University of New South Wales, Sydney, Kensington, NSW, 2052, Australia.

出版信息

Environ Res. 2024 Apr 1;246:118097. doi: 10.1016/j.envres.2024.118097. Epub 2024 Jan 2.

Abstract

This study examined the use of modified multiwall carbon nanotubes (M-MWCNTs) with immobilized laccase (L@M-MWCNTs) for removing ciprofloxacin (Cip), carbamazepine (Cbz), diclofenac (Dcf), benzo[a]pyrene (Bap), and anthracene (Ant) from different water samples. The synthesized materials were characterized using an array of advanced analytical techniques. The physical immobilization of laccase onto M-MWCNTs was confirmed through Scanning electron microscope (SEM)-dispersive X-ray spectroscopy (EDS) analysis and Brunner-Emmet-Teller (BET) surface area measurements. The specific surface area of M-MWCNTs decreased by 65% upon laccase immobilization. There was also an increase in nitrogen content seen by EDS analysis asserting successful immobilization. The results of Boehm titration and Fourier transform infrared (FTIR) exhibited an increase in acidic functional groups after laccase immobilization. L@M-MWCNTs storage for two months maintained 77.8%, 61.6%, and 57.6% of its initial activity for 4 °C, 25 °C, and 35 °C, respectively. In contrast, the free laccase exhibited 55.3%, 37.5%, and 23.5% of its initial activity at 4 °C, 25 °C, and 35 °C, respectively. MWCNTs improved storability and widened the working temperature range of laccase. The optimum removal conditions of studied pollutants were pH 5, 25 °C, and 1.6 g/L of M-MWCNTs. These parameters led to >90% removal of the targeted pollutants for four treatment cycles of both synthetic water and spiked lake water. L@M-MWCNTs demonstrated consistent removal of >90% for up to five cycles even with spiked wastewater. The adsorption was endothermic and followed Langmuir isotherm. Oxidation, dehydrogenation, hydroxylation, and ring cleavage seem to be the dominant degradation mechanisms.

摘要

本研究考察了固定化漆酶的改性多壁碳纳米管(L@M-MWCNTs)用于去除不同水样中 ciprofloxacin(Cip)、carbamazepine(Cbz)、diclofenac(Dcf)、benzo[a]pyrene(Bap)和 anthracene(Ant)的效果。使用一系列先进分析技术对合成材料进行了表征。通过扫描电子显微镜(SEM)-色散X射线光谱(EDS)分析和Brunner-Emmet-Teller(BET)表面积测量,证实了漆酶在M-MWCNTs上的物理固定。漆酶固定后,M-MWCNTs的比表面积下降了65%。EDS分析还显示氮含量增加,表明固定成功。Boehm滴定和傅里叶变换红外(FTIR)结果表明,漆酶固定后酸性官能团增加。L@M-MWCNTs在4℃、25℃和35℃下储存两个月后,分别保持其初始活性的77.8%、61.6%和57.6%。相比之下,游离漆酶在4℃、25℃和35℃下分别仅表现出其初始活性的55.3%、37.5%和23.5%。MWCNTs提高了漆酶的储存稳定性并拓宽了其工作温度范围。所研究污染物的最佳去除条件为pH 5、25℃和1.6 g/L的M-MWCNTs。这些参数使得在合成水和加标湖水的四个处理循环中,目标污染物的去除率>90%。即使对于加标废水,L@M-MWCNTs在多达五个循环中也能保持>90%的一致去除率。吸附是吸热的,且遵循Langmuir等温线。氧化、脱氢、羟基化和环裂解似乎是主要的降解机制。

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