The antifouling properties of traditional self-polishing marine antifouling coatings are mainly achieved based on their hydrolysis-sensitive side groups or the degradable polymer main chains. Here, we prepared a highly branched copolymer for selfpolishing antifouling coatings, in which the primary polymer chains are bridged by degradable fragments (poly-ε-caprolactone, PCL). Owing to the partial or complete degradation of PCL fragments, the remaining coating on the surface can be broken down and eroded by seawater. Finally, the polymeric surface is self-polished and self-renewed. The designed highly branched copolymers were successfully prepared by reversible complexation mediated polymerization (RCMP), and their primary main chains had an M n of approximately 3410 g•mol −1 . The hydrolytic degradation results showed that the degradation of the copolymer was controlled, and the degradation rate increased with increasing contents of degradable fragments. The algae settlement assay tests indicated that the copolymer itself has some antibiofouling ability. Moreover, the copolymer can serve as a controlled release matrix for antifoulant 4,5-dichloro-2-octylisothiazolone (DCOIT), and the release rate increases with the contents of degradable fragments. The marine field tests confirmed that these copolymer-based coatings exhibited excellent antibiofouling ability for more than 3 months. The current copolymer is derived from commonly used monomers and an easily conducted polymerization method. Hence, we believe this method may offer innovative insights into marine antifouling applications.
We reported a facile and effective method for the preparation of highly branched polymers by combining the concepts of self-condensing vinyl polymerization (SCVP) and iodine transfer polymerization (ITP). This procedure used a chain transfer monomer synthesized in situ from a commercially available chloride compound, p-chloromethylstyrene (CMS). The efficiencies of the halogen exchange from the alkyl chloride (−CH2Cl) to the alkyl iodide (−CH2I) at room and high temperature were studied using CMS and benzyl chloride as model halogenated compounds. The structures of the resulting polymer and the branching behavior were analyzed by nuclear magnetic resonance (NMR) spectroscopy and size-exclusion chromatography (SEC) equipped with a differential refractive index detector, a multiangle laser light scattering detector, and a viscometer detector. The model study using small molecules revealed that −CH2Cl could efficiently halogen exchange with sodium iodide (NaI) at both room and high temperature. The model linear polymerization in the presence of benzyl chloride and NaI confirmed the controlled nature of the polymerization. The results of the branched polymerization studies suggested that the degree of branching in the resulting polymers increased as the amount of NaI increased, and the majority of the branching occurred during the last stage of the polymerization. The current work should provide a simple procedure for the synthesis of highly branched polymers from commercially available compounds, and this method could be used for the preparation of various highly branched polymers.
Abstract. This paper reports the rapid synthesis of a dual-responsive copolymer through reversible addition-fragmentation chain transfer (RAFT) polymerization under microwave irradiation. Through use of 2-ethoxycarbonothioylthio acetic acid (ECTA) as a RAFT agent, the microwave-assisted polymerization rate of N-isopropylacrylamide (NIPAM) was approximately 150 times faster than that observed under conventional heating conditions, and the resulting homopolymer can be reactivated as a macroinitiator to produce poly(N-isopropylacrylamide-block-methacrylic acid) (PNIPAM-b-PMAA) block copolymers through a similar method. Research into the detailed polymerization kinetics of the PNIPAM and PNIPAM-b-PMAA revealed living characteristics that included a linear relationship between M n and conversion, controlled molecular weights, and a relatively narrow molecular weight distribution. The solution of the block copolymers in phosphate-buffered saline buffer displayed a phase transition at a lower critical solution temperature transition of 42°C, and altering the pH from 7 to 3.5 resulted in various degrees of polymer aggregation in the solution. Cisplatin was loaded to the polymeric carrier through a ligand exchange to form a macromolecular prodrug. The observed critical micelle concentration was 0.25 mg/mL. Overall, these polymers offer considerable potential for developing a new multifunctional drug delivery system.
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