| Title |
Structural Elucidation of a Metagenomic Urethanase and Its Engineering Towards Enhanced Hydrolysis Profiles |
| ID_Doc |
11134 |
| Authors |
Bayer, T; Palm, GJ; Berndt, L; Meinert, H; Branson, Y; Schmidt, L; Cziegler, C; Somvilla, I; Zurr, C; Graf, LG; Janke, U; Badenhorst, CPS; König, S; Delcea, M; Garscha, U; Wei, R; Lammers, M; Bornscheuer, UT |
| Title |
Structural Elucidation of a Metagenomic Urethanase and Its Engineering Towards Enhanced Hydrolysis Profiles |
| Year |
2024 |
| Published |
|
| DOI |
10.1002/anie.202404492 |
| Abstract |
While plastics like polyethylene terephthalate can already be degraded efficiently by the activity of hydrolases, other synthetic polymers like polyurethanes (PUs) and polyamides (PAs) largely resist biodegradation. In this study, we solved the first crystal structure of the metagenomic urethanase UMG-SP-1, identified highly flexible loop regions to comprise active site residues, and targeted a total of 20 potential hot spots by site-saturation mutagenesis. Engineering campaigns yielded variants with single mutations, exhibiting almost 3- and 8-fold improved activity against highly stable N-aryl urethane and amide bonds, respectively. Furthermore, we demonstrated the release of the corresponding monomers from a thermoplastic polyester-PU and a PA (nylon 6) by the activity of a single, metagenome-derived urethanase after short incubation times. Thereby, we expanded the hydrolysis profile of UMG-SP-1 beyond the reported low-molecular weight carbamates. Together, these findings promise advanced strategies for the bio-based degradation and recycling of plastic materials and waste, aiding efforts to establish a circular economy for synthetic polymers. Plastics like polyurethanes (PUs) and polyamides (PAs) largely resist biodegradation. Herein, we report the first crystal structure of the metagenomic urethanase UMG-SP-1. Subsequent engineering yielded variants with up to 8-fold enhanced activity on various urethanes and amides. UMG-SP-1 variants partially degraded a model thermoplastic polyester-PU and nylon 6, highlighting its applicability for the biodegradation and recycling of PU and PA. image |
| Author Keywords |
amidase; loop engineering; polymers; plastic (bio)degradation; urethanase structure |
| Index Keywords |
Index Keywords |
| Document Type |
Other |
| Open Access |
Open Access |
| Source |
Science Citation Index Expanded (SCI-EXPANDED) |
| EID |
WOS:001291378400001 |
| WoS Category |
Chemistry, Multidisciplinary |
| Research Area |
Chemistry |
| PDF |
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