Efficient Degradation of Tetracycline Antibiotics by Engineered Myoglobin with High Peroxidase Activity
Tetracyclines are one class of widely used antibiotics. Meanwhile, due to abuse and improper disposal, they are often detected in wastewater, which causes a series of environmental problems and poses a threat to human health and safety. As an efficient and environmentally friendly method, enzymatic...
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MDPI AG
2022-12-01
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| Series: | Molecules |
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| author | Guang-Rong Wu Li-Juan Sun Jia-Kun Xu Shu-Qin Gao Xiang-Shi Tan Ying-Wu Lin |
| author_facet | Guang-Rong Wu Li-Juan Sun Jia-Kun Xu Shu-Qin Gao Xiang-Shi Tan Ying-Wu Lin |
| author_sort | Guang-Rong Wu |
| collection | DOAJ |
| description | Tetracyclines are one class of widely used antibiotics. Meanwhile, due to abuse and improper disposal, they are often detected in wastewater, which causes a series of environmental problems and poses a threat to human health and safety. As an efficient and environmentally friendly method, enzymatic catalysis has attracted much attention. In previous studies, we have designed an efficient peroxidase (F43Y/P88W/F138W Mb, termed YWW Mb) based on the protein scaffold of myoglobin (Mb), an O<sub>2</sub> carrier, by modifying the heme active center and introducing two Trp residues. In this study, we further applied it to degrade the tetracycline antibiotics. Both UV-Vis and HPLC studies showed that the triple mutant YWW Mb was able to catalyze the degradation of tetracycline, oxytetracycline, doxycycline, and chlortetracycline effectively, with a degradation rate of ~100%, ~98%, ~94%, and ~90%, respectively, within 5 min by using H<sub>2</sub>O<sub>2</sub> as an oxidant. These activities are much higher than those of wild-type Mb and other heme enzymes such as manganese peroxidase. As further analyzed by UPLC-ESI-MS, we identified multiple degradation products and thus proposed possible degradation mechanisms. In addition, the toxicity of the products was analyzed by using in vitro antibacterial experiments of <i>E. coli</i>. Therefore, this study indicates that the engineered heme enzyme has potential applications for environmental remediation by degradation of tetracycline antibiotics. |
| first_indexed | 2024-03-09T16:03:39Z |
| format | Article |
| id | doaj.art-de63671967994497ac3e156478dcb852 |
| institution | Directory Open Access Journal |
| issn | 1420-3049 |
| language | English |
| last_indexed | 2024-03-09T16:03:39Z |
| publishDate | 2022-12-01 |
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| series | Molecules |
| spelling | doaj.art-de63671967994497ac3e156478dcb8522023-11-24T16:55:15ZengMDPI AGMolecules1420-30492022-12-012724866010.3390/molecules27248660Efficient Degradation of Tetracycline Antibiotics by Engineered Myoglobin with High Peroxidase ActivityGuang-Rong Wu0Li-Juan Sun1Jia-Kun Xu2Shu-Qin Gao3Xiang-Shi Tan4Ying-Wu Lin5School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, ChinaHengyang Medical School, University of South China, Hengyang 421001, ChinaKey Laboratory of Sustainable Development of Polar Fisheries, Yellow Sea Fisheries Research Institute, Chinese Academy of Fishery Sciences, Qingdao 266071, ChinaHengyang Medical School, University of South China, Hengyang 421001, ChinaDepartment of Chemistry & Institute of Biomedical Science, Fudan University, Shanghai 200433, ChinaSchool of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, ChinaTetracyclines are one class of widely used antibiotics. Meanwhile, due to abuse and improper disposal, they are often detected in wastewater, which causes a series of environmental problems and poses a threat to human health and safety. As an efficient and environmentally friendly method, enzymatic catalysis has attracted much attention. In previous studies, we have designed an efficient peroxidase (F43Y/P88W/F138W Mb, termed YWW Mb) based on the protein scaffold of myoglobin (Mb), an O<sub>2</sub> carrier, by modifying the heme active center and introducing two Trp residues. In this study, we further applied it to degrade the tetracycline antibiotics. Both UV-Vis and HPLC studies showed that the triple mutant YWW Mb was able to catalyze the degradation of tetracycline, oxytetracycline, doxycycline, and chlortetracycline effectively, with a degradation rate of ~100%, ~98%, ~94%, and ~90%, respectively, within 5 min by using H<sub>2</sub>O<sub>2</sub> as an oxidant. These activities are much higher than those of wild-type Mb and other heme enzymes such as manganese peroxidase. As further analyzed by UPLC-ESI-MS, we identified multiple degradation products and thus proposed possible degradation mechanisms. In addition, the toxicity of the products was analyzed by using in vitro antibacterial experiments of <i>E. coli</i>. Therefore, this study indicates that the engineered heme enzyme has potential applications for environmental remediation by degradation of tetracycline antibiotics.https://www.mdpi.com/1420-3049/27/24/8660heme enzymemyoglobinantibioticsdegradationenvironmental remediation |
| spellingShingle | Guang-Rong Wu Li-Juan Sun Jia-Kun Xu Shu-Qin Gao Xiang-Shi Tan Ying-Wu Lin Efficient Degradation of Tetracycline Antibiotics by Engineered Myoglobin with High Peroxidase Activity Molecules heme enzyme myoglobin antibiotics degradation environmental remediation |
| title | Efficient Degradation of Tetracycline Antibiotics by Engineered Myoglobin with High Peroxidase Activity |
| title_full | Efficient Degradation of Tetracycline Antibiotics by Engineered Myoglobin with High Peroxidase Activity |
| title_fullStr | Efficient Degradation of Tetracycline Antibiotics by Engineered Myoglobin with High Peroxidase Activity |
| title_full_unstemmed | Efficient Degradation of Tetracycline Antibiotics by Engineered Myoglobin with High Peroxidase Activity |
| title_short | Efficient Degradation of Tetracycline Antibiotics by Engineered Myoglobin with High Peroxidase Activity |
| title_sort | efficient degradation of tetracycline antibiotics by engineered myoglobin with high peroxidase activity |
| topic | heme enzyme myoglobin antibiotics degradation environmental remediation |
| url | https://www.mdpi.com/1420-3049/27/24/8660 |
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