School of Civil Engineering, Architecture and Environment, Hubei University of Technology, Wuhan 430068, China.
Hubei Key Laboratory of Ecological Restoration for River-Lakes and Algal Utilization, Wuhan 430068, China.
Molecules. 2021 Nov 11;26(22):6803. doi: 10.3390/molecules26226803.
The negative impacts on the ecosystem of antibiotic residues in the environment have become a global concern. However, little is known about the transformation mechanism of antibiotics by manganese peroxidase (MnP) from microorganisms. This work investigated the transformation characteristics, the antibacterial activity of byproducts, and the degradation mechanism of tetracycline (TC) by purified MnP from . The results show that nitrogen-limited and high level of Mn medium could obtain favorable MnP activity and inhibit the expression of lignin peroxidase by . The purified MnP could transform 80% tetracycline in 3 h, and the threshold of reaction activator (HO) was about 0.045 mmol L. After the 3rd cyclic run, the transformation rate was almost identical at the low initial concentration of TC (77.05-88.47%), while it decreased when the initial concentration was higher (49.36-60.00%). The antimicrobial potency of the TC transformation products by MnP decreased throughout reaction time. We identified seven possible degradation products and then proposed a potential TC transformation pathway, which included demethylation, oxidation of the dimethyl amino, decarbonylation, hydroxylation, and oxidative dehydrogenation. These findings provide a novel comprehension of the role of MnP on the fate of antibiotics in nature and may develop a potential technology for tetracycline removal.
抗生素残留对生态系统的负面影响已成为全球关注的焦点。然而,人们对于微生物来源的锰过氧化物酶(MnP)转化抗生素的机制知之甚少。本研究旨在探讨从 中分离纯化的 MnP 对四环素(TC)的转化特性、副产物的抑菌活性以及降解机制。结果表明,氮限制和高 Mn 培养基可以获得较高的 MnP 活性,并抑制 的木质素过氧化物酶的表达。纯化的 MnP 可以在 3 h 内转化 80%的四环素,反应激活剂(HO)的阈值约为 0.045 mmol/L。在第 3 次循环运行后,当 TC 的初始浓度较低(77.05%-88.47%)时,转化速率几乎相同,但当初始浓度较高时,转化速率下降(49.36%-60.00%)。MnP 转化产物的抑菌活性随反应时间的延长而降低。我们鉴定了七种可能的降解产物,并提出了一种潜在的 TC 转化途径,该途径包括去甲基化、二甲氨基氧化、脱羰基、羟化和氧化脱氢。这些发现为 MnP 对自然界中抗生素命运的作用提供了新的认识,并可能为四环素的去除开发出一种潜在的技术。