PMID- 34743799 OWN - NLM STAT- MEDLINE DCOM- 20220125 LR - 20220125 IS - 1879-1298 (Electronic) IS - 0045-6535 (Linking) VI - 291 IP - Pt 1 DP - 2022 Mar TI - A robust biocatalyst based on laccase immobilized superparamagnetic Fe(3)O(4)@SiO(2)-NH(2) nanoparticles and its application for degradation of chlorophenols. PG - 132727 LID - S0045-6535(21)03199-4 [pii] LID - 10.1016/j.chemosphere.2021.132727 [doi] AB - The presence of chlorophenols in water and wastewater is considered a serious environmental issue. To eliminate these micropollutants, biodegradation of chlorophenols using enzyme-nanoparticle conjugated biocatalyst, is proposed as an economical and eco-friendly method. Herein, amino-functionalized superparamagnetic Fe(3)O(4)@SiO(2)-NH(2) nanoparticles with core-shell structure were constructed as a promising carrier for immobilization of laccase from Trametes versicolor. Compared with free laccase, Fe(3)O(4)@SiO(2)-NH(2)-Laccase displayed remarkable outcomes in all major areas such as temperature and storage stabilities, and tolerance to organic solvents and metal ions. The biocatalytic performance and reusability of Fe(3)O(4)@SiO(2)-NH(2)-Laccase were evaluated for the degradation of 2,4-dichlorophenol (2,4-DCP) and 2,4,6-trichlorophenol (2,4,6-TCP) in repeated cycles. Even after 10 successive reuses, the degradation rate of 2,4-DCP and 2,4,6-TCP were found to be 54.9% and 68.7%, respectively. The influences of solution pH, initial chlorophenol concentration, and temperature on the degradation rate of these two chlorophenols were evaluated. The degradation intermediate products including dimers, trimers, and tetramers of 2,4-DCP and 2,4,6-TCP were identified. Release of chloride ions was observed during the enzymatic degradation of these two chlorophenols. Based on the determination of intermediate products and released chloride ions, the degradation pathway that was involved in dehydrogenation, reactive radical intermediates formation, dechlorination, self-coupling and oligomers/polymers formation was proposed. The toxicity of these two chlorophenols and their intermediates was substantially reduced during the enzymatic degradation. The results of this study might present an alternative clean biotechnology for the remediation of 2,4-DCP and 2,4,6-TCP contaminated water matrices. CI - Copyright (c) 2021 Elsevier Ltd. All rights reserved. FAU - Chen, Zhihui AU - Chen Z AD - School of Water Resources and Environment, China University of Geosciences (Beijing), 29 Xueyuan Road, Haidian District, 100083, Beijing, China. FAU - Yao, Jun AU - Yao J AD - School of Water Resources and Environment, China University of Geosciences (Beijing), 29 Xueyuan Road, Haidian District, 100083, Beijing, China. Electronic address: yaojun@cugb.edu.cn. FAU - Ma, Bo AU - Ma B AD - School of Water Resources and Environment, China University of Geosciences (Beijing), 29 Xueyuan Road, Haidian District, 100083, Beijing, China. FAU - Liu, Bang AU - Liu B AD - School of Water Resources and Environment, China University of Geosciences (Beijing), 29 Xueyuan Road, Haidian District, 100083, Beijing, China. FAU - Kim, Jonghyok AU - Kim J AD - School of Water Resources and Environment, China University of Geosciences (Beijing), 29 Xueyuan Road, Haidian District, 100083, Beijing, China. FAU - Li, Hao AU - Li H AD - School of Water Resources and Environment, China University of Geosciences (Beijing), 29 Xueyuan Road, Haidian District, 100083, Beijing, China. FAU - Zhu, Xiaozhe AU - Zhu X AD - School of Water Resources and Environment, China University of Geosciences (Beijing), 29 Xueyuan Road, Haidian District, 100083, Beijing, China. FAU - Zhao, Chenchen AU - Zhao C AD - School of Water Resources and Environment, China University of Geosciences (Beijing), 29 Xueyuan Road, Haidian District, 100083, Beijing, China. FAU - Amde, Meseret AU - Amde M AD - School of Water Resources and Environment, China University of Geosciences (Beijing), 29 Xueyuan Road, Haidian District, 100083, Beijing, China; Department of Chemistry, College of Natural and Computational Sciences, Haramaya University, Oromia, Ethiopia. LA - eng PT - Journal Article DEP - 20211028 PL - England TA - Chemosphere JT - Chemosphere JID - 0320657 RN - 0 (Chlorophenols) RN - 0 (Enzymes, Immobilized) RN - 7631-86-9 (Silicon Dioxide) RN - EC 1.10.3.2 (Laccase) SB - IM MH - *Chlorophenols MH - Enzymes, Immobilized MH - Laccase MH - Magnetic Iron Oxide Nanoparticles MH - *Nanoparticles MH - Silicon Dioxide MH - Trametes OTO - NOTNLM OT - Chlorophenols OT - Dechlorination OT - Degradation mechanism OT - Laccase immobilization OT - Reusability OT - Toxicity EDAT- 2021/11/09 06:00 MHDA- 2022/01/27 06:00 CRDT- 2021/11/08 05:39 PHST- 2021/07/19 00:00 [received] PHST- 2021/10/23 00:00 [revised] PHST- 2021/10/26 00:00 [accepted] PHST- 2021/11/09 06:00 [pubmed] PHST- 2022/01/27 06:00 [medline] PHST- 2021/11/08 05:39 [entrez] AID - S0045-6535(21)03199-4 [pii] AID - 10.1016/j.chemosphere.2021.132727 [doi] PST - ppublish SO - Chemosphere. 2022 Mar;291(Pt 1):132727. doi: 10.1016/j.chemosphere.2021.132727. Epub 2021 Oct 28.