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Multilayer Engineering of Enzyme Cascade Catalysis for One-Pot Preparation of Nylon Monomers from Renewable Fatty Acids

Title
Multilayer Engineering of Enzyme Cascade Catalysis for One-Pot Preparation of Nylon Monomers from Renewable Fatty Acids
Authors
Kim, Tae-HunKang, Su-HwanHan, Jeong-EunSeo, Eun-JiJeon, Eun-YeongChoi, Go-EunPark, Jin-ByungOh, Deok-Kun
Ewha Authors
여창열박진병
SCOPUS Author ID
여창열scopus; 박진병scopus
Issue Date
2020
Journal Title
ACS CATALYSIS
ISSN
2155-5435JCR Link
Citation
ACS CATALYSIS vol. 10, no. 9, pp. 4871 - 4878
Keywords
multilayer engineeringone-pot preparationC11 nylon monomersricinoleic acidmaltose-binding proteinfusion enzymecofactor regenerationresin adsorption
Publisher
AMER CHEMICAL SOC
Indexed
SCIE; SCOPUS WOS scopus
Document Type
Article
Abstract
Enzyme cascade catalysis has critical problems in obtaining the high concentrations of products, such as the low stabilities and activities of biocatalysts and the inhibition by hydrophobic reactants at high concentrations to biocatalysts. Here, we performed multilayer engineering of enzyme cascade catalysis to produce C11 nylon monomers at commercially viable concentrations from ricinoleic acid. The catalysis was driven by engineered Escherichia coli-based whole-cell biocatalysts and cell-free enzymes (i.e., lipases). Stabilities and activities of the biocatalysts were improved by engineering the bottleneck enzyme Baeyer-Villiger monooxygenase and introducing a cofactor regeneration system. The inhibitory effects of the byproducts n-heptanoic acid and pyruvate on the cascade enzymes were overcome, and the products were simply recovered in situ by engineering of reactions with the addition of an adsorbent resin. We obtained 248 mM undecanedioic acid or 232 mM 11-aminoundecanoic acid as a nylon monomer from 300 mM ricinoleic acid by multilayer engineering. The concentration was 500- and 640-fold higher than those produced by nonengineering, respectively. We have also simply isolated the C11 nylon monomers via solvent extraction to a rather high purity. This study will contribute to the industrial enzyme cascade synthesis of nylon monomers in an environmentally-friendly route from renewable biomass.
DOI
10.1021/acscatal.9b05426
Appears in Collections:
자연과학대학 > 생명과학전공 > Journal papers
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