Abstract:
:A unified kinetic pathway for the enzyme-catalyzed polymerization and degradation of poly(ε-caprolactone) was developed. This model tracks the complete distribution of individual chain lengths, both enzyme-bound and in solution, and successfully predicts monomer conversion and the molecular mass distribution as a function of reaction time. As compared to reported experimental data for polymerization reactions, modeled kinetics generate similar trends, with ring-opening rates and water concentration as key factors to controlling molecular mass distributions. Water is critically important by dictating the number of linear chains in solution, shifting the molecular mass distribution at which propagation and degradation equilibrate. For the enzymatic degradation of poly(ε-caprolactone), the final reaction product is also consistent with the equilibrium dictated by the propagation and degradation rates. When the modeling framework described here is used, further experiments can be designed to isolate key reaction steps and provide methods for improving the efficiency of enzyme polymerization.
journal_name
Biomacromoleculesjournal_title
Biomacromoleculesauthors
Johnson PM,Kundu S,Beers KLdoi
10.1021/bm2009312subject
Has Abstractpub_date
2011-09-12 00:00:00pages
3337-43issue
9eissn
1525-7797issn
1526-4602journal_volume
12pub_type
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