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Improving the catalytic efficiency and stereoselectivity of a nitrilase from Synechocystis sp. PCC6803 by semi-rational engineering en route to chiral γ-amino acids

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논문

Improving the catalytic efficiency and stereoselectivity of a nitrilase from Synechocystis sp. PCC6803 by semi-rational engineering en route to chiral γ-amino acids

학술지

Catalysis science & technology

저자명

Yu, Shanshan; Yao, Peiyuan; Li, Jinlong; Feng, Jinhui; Wu, Qiaqing; Zhu, Dunming

초록

<P>Nitrilase-catalysed desymmetrization of 3-substituted glutaronitriles to optically active 3-substituted 4-cyanobutanoic acid offers an attractive approach to access chiral &beta;-substituted &gamma;-amino acids, an important moiety in pharmaceuticals. In this study, we employed enzyme-substrate docking and alanine scanning to determine the key amino acid residues which have a positive effect on the activity and stereoselectivity of a nitrilase from <I>Synechocystis</I> sp. PCC6803 (<I>Ss</I>NIT). Then, site-saturation mutagenesis and combinatorial mutagenesis of the positive amino acid residues (H141, P194, M197, I201 and F202) were performed, and a double mutant (P194A/F202V) and a triple mutant (P194A/I201A/F202V) with high activity and stereoselectivity were identified for desymmetrization of 3-substituted glutaronitriles to afford (<I>S</I>)-3-substituted-4-cyanobutanoic acids with a high space-time productivity of up to 488 g L<SUP>&#x2212;1</SUP> d<SUP>&#x2212;1</SUP>. Molecular calculation suggests that the enzymatic activity improvement may be due to the enlargement of the substrate binding cavity. It is interesting that the stereoselectivity is enhanced simultaneously.</P>

발행연도

2019

발행기관

The Royal Society of Chemistry

ISSN

2044-4753

ISSN

2044-4761

9

6

페이지

pp.1504-1510

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논문; 2019-12-31

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