One-Pot Microbial Production, Mechanical Properties, and Enzymatic Degradation of Isotactic P[(R)-2-hydroxybutyrate] and Its Copolymer with (R)-Lactate

被引:34
作者
Matsumoto, Ken'ichiro [1 ,2 ]
Terai, Satsuki [1 ]
Ishiyama, Ayako [1 ]
Sun, Jian [1 ]
Kabe, Taizo [2 ,3 ]
Song, Yuyang [1 ]
Nduko, John Masani [1 ]
Iwata, Tadahisa [2 ,3 ]
Taguchi, Seiichi [1 ,2 ]
机构
[1] Hokkaido Univ, Div Biotechnol & Macromol Chem, Grad Sch Engn, Kita Ku, Sapporo, Hokkaido 0608628, Japan
[2] Japan Sci & Technol Agcy, CREST, Kawaguchi, Saitama 3320012, Japan
[3] Univ Tokyo, Grad Sch Agr & Life Sci, Bunkyo Ku, Tokyo 1138657, Japan
关键词
ESCHERICHIA-COLI; SUBSTITUTED POLY(LACTIDE)S; POLYESTERS; BIOSYNTHESIS; POLYLACTIDES; SYNTHASES; ACID);
D O I
10.1021/bm400278j
中图分类号
Q5 [生物化学]; Q7 [分子生物学];
学科分类号
071010 ; 081704 ;
摘要
P[(R)-2-hydroxybutyrate] [P((R)-2HB)] is an aliphatic polyester analogous to poly(lactic acid) (PLA). However, little has been known for its properties because of a high cost of commercially available chiral 2HB as a starting substance for chemical polymer synthesis. In this study, P[(R)-2HB] and P[(R)-2HB-co-(R)-lactate] [P((R)-2HB-co-(R)-LA)] with a new monomer combination were successfully synthesized in recombinant Escherichia coli LS5218 from less-expensive racemic 2HB using an R-specific polyester synthase. The cells expressing an engineered polyhydroxyalkanoate synthase from Pseudomonas sp. 61-3 and propionyl-CoA transferase from Megasphaera elsdenii were grown on LB medium containing 2HB and glucose in a shake flask and accumulated up to 17 wt% of P[(R)-2HB] with optical purity of >99.1%. In addition, the same cells cultured in a jar-fermentor produced P(86 mol% 2HB-co-LA) copolymer. Notably, the molecular weights (M-w) of P(2HB) (27000) and P(2HB-co-LA) (39000) were 2- and 3-fold higher than that of P(2HB) previously synthesized by chemical polycondensation. P(2HB) was processed into a transparent film by solvent-casting and it had flexible properties with elongation at break of 173%, which was contrast to the rigid PLA. Regarding mechanical properties, P(2HB-co-LA) was tougher but less stretchy than P(2HB). These results demonstrated that P(2HB) has useful properties and LA units in 2HB-based polymers can act as a controllable modulator of the material properties. In addition, P[(R)-2HB] was efficiently degraded by treatment of Novozym 42044 (lipase) but not Savinase 16L (protease), indicating that the degrading behavior of the polymer was similar to that of P[(R)-LA].
引用
收藏
页码:1913 / 1918
页数:6
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