Abstract
Polymerization reactions are commonly effected by exposing monomer formulations to some initiation stimulus such as elevated temperature, light, or a chemical reactant. Increasingly, these polymerization reactions are mediated by enzymes―catalytic proteins―owing to their reaction efficiency under mild conditions as well as their environmental friendliness. The utilization of enzymes, particularly oxidases and peroxidases, for generating radicals via reduction-oxidation mechanisms is especially common for initiating radical-mediated polymerization reactions, including vinyl chain-growth polymerization, atom transfer radical polymerization, thiol–ene step-growth polymerization, and polymerization via oxidative coupling. While enzyme-mediated polymerization is useful for the production of materials intended for subsequent use, it is especially well-suited for in situ polymerizations, where the polymer is formed in the place where it will be utilized. Such polymerizations are especially useful for biomedical adhesives and for sensing applications.
Highlights
Synthetically-generated polymers are used in countless applications, from industrial paints, coatings, and sealants, to plastics utilized in automotive and aerospace industries, to biomedical materials such as surgical glues or dental fillings
In the results provided by Lalot, no polymerization proceeded in the absence of the mediator and would, as noted above, start immediately upon its addition [31]; delaying the addition of the mediator permitted the hydrogen peroxide to degrade HRP, leading to a significant decrease in yield
The utilization of HRP for either vinyl polymerization or oxidative coupling has many similarities, including a tendency for HRP to be deactivated by excess hydrogen peroxide; one strategy to inhibit HRP-deactivation was to add poly(ethylene glycol) as it seemed to offer some protection to the enzyme and extended its useful lifetime [25]
Summary
Synthetically-generated polymers are used in countless applications, from industrial paints, coatings, and sealants, to plastics utilized in automotive and aerospace industries, to biomedical materials such as surgical glues or dental fillings. Though certainly not all [3,4,5,6,7,8,9], enzyme-mediated polymerization reactions involve free radicals; these free radical species are generated either directly by the enzyme or via a secondary reaction involving an enzyme-derived product, methods that eliminate the requirement for the thermal energy or irradiation used to initiate conventional free radical polymerization. These enzymatic, radical-generating reactions all utilize reduction and oxidation steps and, most of the enzymes used in these processes are termed oxidoreductases. These three enzymes, as well as several others with similar behavior, are able to initiate, catalyze, or otherwise influence polymerization reactions
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