دورية أكاديمية

Natural diversity screening, assay development, and characterization of nylon-6 enzymatic depolymerization.

التفاصيل البيبلوغرافية
العنوان: Natural diversity screening, assay development, and characterization of nylon-6 enzymatic depolymerization.
المؤلفون: Bell EL; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO, 80401, USA.; BOTTLE Consortium, Golden, CO, 80401, USA., Rosetto G; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO, 80401, USA., Ingraham MA; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO, 80401, USA.; BOTTLE Consortium, Golden, CO, 80401, USA., Ramirez KJ; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO, 80401, USA.; BOTTLE Consortium, Golden, CO, 80401, USA., Lincoln C; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO, 80401, USA.; BOTTLE Consortium, Golden, CO, 80401, USA., Clarke RW; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO, 80401, USA.; BOTTLE Consortium, Golden, CO, 80401, USA., Gado JE; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO, 80401, USA.; BOTTLE Consortium, Golden, CO, 80401, USA., Lilly JL; Battelle Memorial Institute, Columbus, OH, 43201, USA., Kucharzyk KH; Battelle Memorial Institute, Columbus, OH, 43201, USA., Erickson E; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO, 80401, USA.; BOTTLE Consortium, Golden, CO, 80401, USA., Beckham GT; Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, CO, 80401, USA. gregg.beckham@nrel.gov.; BOTTLE Consortium, Golden, CO, 80401, USA. gregg.beckham@nrel.gov.
المصدر: Nature communications [Nat Commun] 2024 Feb 09; Vol. 15 (1), pp. 1217. Date of Electronic Publication: 2024 Feb 09.
نوع المنشور: Journal Article
اللغة: English
بيانات الدورية: Publisher: Nature Pub. Group Country of Publication: England NLM ID: 101528555 Publication Model: Electronic Cited Medium: Internet ISSN: 2041-1723 (Electronic) Linking ISSN: 20411723 NLM ISO Abbreviation: Nat Commun Subsets: MEDLINE
أسماء مطبوعة: Original Publication: [London] : Nature Pub. Group
مواضيع طبية MeSH: Nylons* , Polymers*/chemistry, Caprolactam/*analogs & derivatives, Hydrolysis ; Polyesters
مستخلص: Successes in biocatalytic polyester recycling have raised the possibility of deconstructing alternative polymers enzymatically, with polyamide (PA) being a logical target due to the array of amide-cleaving enzymes present in nature. Here, we screen 40 potential natural and engineered nylon-hydrolyzing enzymes (nylonases), using mass spectrometry to quantify eight compounds resulting from enzymatic nylon-6 (PA6) hydrolysis. Comparative time-course reactions incubated at 40-70 °C showcase enzyme-dependent variations in product distributions and extent of PA6 film depolymerization, with significant nylon deconstruction activity appearing rare. The most active nylonase, a NylC K variant we rationally thermostabilized (an N-terminal nucleophile (Ntn) hydrolase, NylC K -TS, T m  = 87.4 °C, 16.4 °C higher than the wild-type), hydrolyzes 0.67 wt% of a PA6 film. Reactions fail to restart after fresh enzyme addition, indicating that substrate-based limitations, such as restricted enzyme access to hydrolysable bonds, prohibit more extensive deconstruction. Overall, this study expands our understanding of nylonase activity distribution, indicates that Ntn hydrolases may have the greatest potential for further development, and identifies key targets for progressing PA6 enzymatic depolymerization, including improving enzyme activity, product selectivity, and enhancing polymer accessibility.
(© 2024. The Author(s).)
References: Nat Commun. 2015 Dec 07;6:10008. (PMID: 26639611)
Nat Commun. 2023 Jul 28;14(1):4556. (PMID: 37507390)
Chemosphere. 2007 May;67(10):2089-95. (PMID: 17257652)
Nat Commun. 2018 Nov 29;9(1):5053. (PMID: 30498220)
Angew Chem Int Ed Engl. 2023 Feb 20;62(9):e202216220. (PMID: 36591907)
N Biotechnol. 2022 Jul 25;69:28-35. (PMID: 35247624)
Biosci Biotechnol Biochem. 2008 Aug;72(8):2141-50. (PMID: 18685217)
Int J Mol Sci. 2022 Aug 23;23(17):. (PMID: 36076913)
Biotechnol Adv. 2021 Nov 15;52:107811. (PMID: 34333090)
Appl Environ Microbiol. 2018 Apr 2;84(8):. (PMID: 29427431)
Mol Biol Evol. 2020 Apr 1;37(4):1237-1239. (PMID: 31904846)
Biotechnol J. 2011 Oct;6(10):1230-9. (PMID: 21751386)
Comput Appl Biosci. 1992 Jun;8(3):275-82. (PMID: 1633570)
Chembiochem. 2023 Feb 1;24(3):e202200516. (PMID: 36399069)
Biotechnol Bioeng. 2013 Oct;110(10):2581-90. (PMID: 23592055)
Mol Biol Evol. 2018 Jun 1;35(6):1547-1549. (PMID: 29722887)
FEBS J. 2023 Jul;290(13):3400-3421. (PMID: 36799721)
J Biochem Biophys Methods. 2006 Nov 30;69(1-2):89-99. (PMID: 16624419)
Adv Sci (Weinh). 2019 May 20;6(14):1900491. (PMID: 31380212)
ACS Catal. 2022 Mar 18;12(6):3382-3396. (PMID: 35368328)
Chem Rev. 2023 May 10;123(9):5612-5701. (PMID: 36916764)
Eur J Biochem. 1991 Aug 15;200(1):165-9. (PMID: 1879421)
Appl Microbiol Biotechnol. 2005 Jun;67(6):778-88. (PMID: 15968570)
Sci Rep. 2018 Jun 27;8(1):9725. (PMID: 29950566)
Chem Rev. 2015 Feb 11;115(3):1308-448. (PMID: 25629559)
Appl Environ Microbiol. 1993 Nov;59(11):3978-80. (PMID: 8285701)
Nucleic Acids Res. 2023 Jan 6;51(D1):D523-D531. (PMID: 36408920)
Appl Environ Microbiol. 1998 Apr;64(4):1366-71. (PMID: 9546174)
ACS Synth Biol. 2016 Jan 15;5(1):65-73. (PMID: 26511532)
Nat Commun. 2022 Dec 21;13(1):7850. (PMID: 36543766)
Biotechnol Bioeng. 2016 Aug;113(8):1658-65. (PMID: 26804057)
J Biotechnol. 2007 Mar 10;128(4):849-57. (PMID: 17306400)
Acta Crystallogr Sect F Struct Biol Cryst Commun. 2005 Oct 1;61(Pt 10):928-30. (PMID: 16511198)
J Biomed Mater Res. 1987 Aug;21(8):991-1003. (PMID: 2958461)
Angew Chem Int Ed Engl. 2020 Sep 1;59(36):15402-15423. (PMID: 32160372)
J Bacteriol. 1992 Dec;174(24):7948-53. (PMID: 1459943)
Angew Chem Int Ed Engl. 2023 Jan 23;62(4):e202212543. (PMID: 36441664)
Polymers (Basel). 2022 Jan 20;14(3):. (PMID: 35160402)
Biotechnol Bioeng. 2009 Mar 1;102(4):1003-11. (PMID: 18942140)
Biotechnol Lett. 2003 Oct;25(20):1743-6. (PMID: 14626419)
J Biol Chem. 2012 Feb 10;287(7):5079-90. (PMID: 22187439)
Nature. 1992 Apr 16;356(6370):615-8. (PMID: 1560844)
Biochemistry. 2018 Sep 11;57(36):5289-5300. (PMID: 30110540)
Nucleic Acids Res. 2021 Jul 2;49(W1):W293-W296. (PMID: 33885785)
Protein Sci. 2009 Aug;18(8):1662-73. (PMID: 19521995)
Appl Environ Microbiol. 2007 Nov;73(21):7099-102. (PMID: 17827307)
ChemSusChem. 2022 Jan 10;15(1):e202101932. (PMID: 34587366)
ACS Catal. 2023 Sep 26;13(20):13156-13166. (PMID: 37881793)
Sci Rep. 2021 Jan 13;11(1):928. (PMID: 33441590)
Proc Natl Acad Sci U S A. 2018 May 8;115(19):E4350-E4357. (PMID: 29666242)
J Biol Chem. 2010 Jan 8;285(2):1239-48. (PMID: 19889645)
Sci Rep. 2019 Nov 5;9(1):16038. (PMID: 31690819)
Nature. 2020 Apr;580(7802):216-219. (PMID: 32269349)
Bioorg Med Chem. 2014 Apr 1;22(7):2220-35. (PMID: 24602400)
Appl Microbiol Biotechnol. 2014 Oct;98(20):8751-61. (PMID: 24962117)
J Am Chem Soc. 2020 Aug 19;142(33):14267-14275. (PMID: 32706584)
Science. 2016 Mar 11;351(6278):1196-9. (PMID: 26965627)
Appl Environ Microbiol. 1997 Jan;63(1):329-31. (PMID: 8979361)
Environ Sci Technol. 2018 Nov 6;52(21):12388-12401. (PMID: 30284819)
Angew Chem Int Ed Engl. 2023 Dec 21;62(52):e202309305. (PMID: 37651344)
المشرفين على المادة: 25038-54-4 (nylon 6)
0 (Nylons)
0 (Polymers)
0 (Polyesters)
6879X594Z8 (Caprolactam)
تواريخ الأحداث: Date Created: 20240209 Date Completed: 20240214 Latest Revision: 20240214
رمز التحديث: 20240214
مُعرف محوري في PubMed: PMC10858056
DOI: 10.1038/s41467-024-45523-5
PMID: 38336849
قاعدة البيانات: MEDLINE
الوصف
تدمد:2041-1723
DOI:10.1038/s41467-024-45523-5