End-Group Analysis of Bacterially Produced Poly(3-hydroxybutyrate): Discovery of Succinate as the Polymerization Starter

The end groups of bacterial poly(3-hydroxybutyrate) (PHB) were analyzed by 1H and 31P NMR spectroscopy and matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS). A PHB component having a molecular weight around 200 000 Da was broken down into low-molecular-weigh...

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Bibliographic Details
Published in:Macromolecules 2009-06, Vol.42 (12), p.4038-4046
Main Authors: Yamanaka, Kenji, Kimura, Yoshiharu, Aoki, Takashi, Kudo, Toshiji
Format: Article
Language:English
Subjects:
Applied sciences
Bioconversions. Hemisynthesis
Biological and medical sciences
Biotechnology
Exact sciences and technology
Fundamental and applied biological sciences. Psychology
Methods. Procedures. Technologies
Organic polymers
Physicochemistry of polymers
Properties and characterization
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Summary:The end groups of bacterial poly(3-hydroxybutyrate) (PHB) were analyzed by 1H and 31P NMR spectroscopy and matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS). A PHB component having a molecular weight around 200 000 Da was broken down into low-molecular-weight oligomers by acid-catalyzed partial hydrolysis. MALDI-TOF MS showed that one series of fragments contain a common terminal group that originated from the primer used for initiating in vivo polymerization. Analysis of the fragments proved that the terminal group is succinate. On the basis of this result, a plausible mechanism is proposed for enzymatic polymerization in microbial PHB synthesis.
ISSN:0024-9297
1520-5835
DOI:10.1021/ma900427z