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重组红曲霉过氧化物酶催化废水中氯四环素的高效、快速和稳定降解。

Efficient, fast and robust degradation of chlortetracycline in wastewater catalyzed by recombinant Arthromyces ramosus peroxidase.

机构信息

School of Medicine, Guangxi University of Science and Technology, Liushi Road 257, Liuzhou 545025, China; Department of Molecular Biosciences and Bioengineering, University of Hawaii at Manoa, 1955 East-West Road, Honolulu, HI 96822, USA.

Department of Molecular Biosciences and Bioengineering, University of Hawaii at Manoa, 1955 East-West Road, Honolulu, HI 96822, USA.

出版信息

Sci Total Environ. 2023 Feb 1;858(Pt 1):159872. doi: 10.1016/j.scitotenv.2022.159872. Epub 2022 Oct 29.

Abstract

Chlortetracycline (CTC), a widely used antibiotic, is recalcitrant and ubiquitous in the environment. Enzymatic degradation of CTC is an economical and efficient bioremediation method. In this work, recombinant Arthromyces ramosus peroxidase (rARP) at a concentration of 3.13 × 10 M was used to catalyze rapid degradation of CTC in water. The second-order rate constants of rARP showed up to 62-fold catalytic efficiency of horseradish peroxidase (HRP) toward CTC. The degradation half-life of CTC at the concentrations of 2 and 40 mg L in wastewater under the rARP catalysis was, respectively, 5.3 and 5.7 min at 25 °C, and 2.7 and 3.1 min at 40 °C, which were up to 15-fold and 111-fold faster than HRP and laccase, respectively, but use of 3 % the amount of rARP as HRP. rARP catalyzed degradation of CTC at 2-40 mg L in wastewater completed in 20-24 min, and its catalytic efficiency varied within only 2-fold at 25-40 °C. rARP showed only 2-3-fold discrepancy of catalytic efficiency among pH 5.0, 7.5 and 9.0. CTC under rARP catalysis underwent demethylation and oxidation to form nontoxic N-dedimethyl-9-hydroxy-CTC. The high catalytic efficiency of rARP agreed with a short distance between rARP's δN-His and CTC's dimethylamine N as indicated by docking simulation. rARP is a useful enzyme for CTC bioremediation.

摘要

金霉素(CTC)是一种广泛使用的抗生素,在环境中具有抗降解性和普遍性。酶促降解 CTC 是一种经济有效的生物修复方法。在这项工作中,浓度为 3.13×10 M 的重组干酪乳杆菌过氧化物酶(rARP)用于催化水中 CTC 的快速降解。rARP 对 CTC 的二级反应速率常数表现出比辣根过氧化物酶(HRP)高达 62 倍的催化效率。在 rARP 催化下,浓度为 2 和 40 mg·L 的废水在 25°C 下的 CTC 半衰期分别为 5.3 和 5.7 min,在 40°C 下分别为 2.7 和 3.1 min,分别比 HRP 和漆酶快 15 倍和 111 倍,但 rARP 的用量仅为 HRP 的 3%。rARP 可在 2-40 mg·L 的废水中在 20-24 min 内完成 CTC 的催化降解,其催化效率在 25-40°C 内仅相差 2 倍。rARP 在 pH 5.0、7.5 和 9.0 之间的催化效率差异仅为 2-3 倍。rARP 催化下的 CTC 经历脱甲基和氧化作用,形成无毒的 N-脱二甲基-9-羟基 CTC。rARP 的高催化效率与对接模拟所示的 rARP 的 δN-His 与 CTC 的二甲胺 N 之间的短距离一致。rARP 是一种用于 CTC 生物修复的有用酶。

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