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Imprinting of metal receptors into multilayer polyelectrolyte films: fabrication and applications in marine antifouling.

ABSTRACT: Polymeric films constructed using the layer-by-layer (LbL) fabrication process were employed as a platform for metal ion immobilization and applied as a marine antifouling coating. The novel Cu²⁺ ion imprinting process described is based on the use of metal ion templates and LbL multilayer covalent cross-linking. Custom synthesized, peptide mimicking polycations composed of histidine grafted poly(allylamine) (PAH) to bind metal ions, and methyl ester containing polyanions for convenient cross-linking were used in the fabrication process. Two methods of LbL film formation have been investigated using alternate polyelectrolyte deposition namely non-imprinted LbL_A, and imprinted LbL_B. Both LbL films were cross linked at mild temperature to yield covalent bridging of the layers for improved stability in a sea water environment. A comparative study of the non-imprinted LbL_A films and imprinted LbL_B films for Cu²⁺ ion binding capacity, leaching rate and stability of the films was performed. The results reveal that the imprinted films possess enhanced affinity to retain metal ions due to the preorganization of imidazole bearing histidine receptors. As a result the binding capacity of the films for Cu²⁺ could be improved by seven fold. Antifouling properties of the resulting materials in a marine environment have been demonstrated against the settlement of barnacle larvae, indicating that controlled release of Cu ions was achieved.

SUBMITTER: Puniredd SR

PROVIDER: S-EPMC5586206 | biostudies-literature | 2015 Jan

REPOSITORIES: biostudies-literature

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Imprinting of metal receptors into multilayer polyelectrolyte films: fabrication and applications in marine antifouling.

Puniredd Sreenivasa Reddy SR Jańczewski Dominik D Go Dewi Pitrasari DP Zhu Xiaoying X Guo Shifeng S Ming Teo Serena Lay SL Chen Lee Serina Siew SS Vancso G Julius GJ

Chemical science 20140926 1

Polymeric films constructed using the layer-by-layer (LbL) fabrication process were employed as a platform for metal ion immobilization and applied as a marine antifouling coating. The novel Cu<sup>2+</sup> ion imprinting process described is based on the use of metal ion templates and LbL multilayer covalent cross-linking. Custom synthesized, peptide mimicking polycations composed of histidine grafted poly(allylamine) (PAH) to bind metal ions, and methyl ester containing polyanions for convenie ...[more]

PMID: 28966763

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Project description:The layer-by-layer film deposition is a suitable strategy for the design and functionalization of drug carriers with superior performance, which still lacks information describing the influence of assembly conditions on the mechanisms governing the drug release process. Herein, traditional poly(acrylic acid)/poly(allylamine) polyelectrolyte multilayers (PEM) were explored as a platform to study the influence of the assembly conditions such as pH, drug loading method, and capping layer deposition on the mechanisms that control the release of calcein, the chosen model drug, from PEM. Films with 20-40 bilayers were assembled at pH 4.5 or 8.8, and the drug loading process was carried out during- or post-film assembly. Release data were fitted to three release models, namely, Higuchi, Ritger-Peppas, and Berens-Hopfenberg, to investigate the mechanism governing the drug transport, such as the apparent diffusion and the relaxation time. The postassembly drug loading method leads to a higher drug loading capacity than the during-assembly method, attributed to the washing out of calcein during film assembly steps in the latter method. Higuchi's and Ritger-Peppas' model analyses indicate that the release kinetic constant increased with the number of bilayers for the postassembly method. The opposite trend is observed for the during-assembly method. The Berens-Hopfenberg release model enabled the decoupling of each drug transport mechanism's contribution, indicating the increase of the diffusion contribution with the number of bilayers for the postassembly method at pH 4.5 and the increase of the polymer relaxation contribution for the during-assembly method at pH 8.8. Deborah's number, which represents the ratio of the polymer relaxation time to the diffusion time, follows the trends observed for the relaxation contribution for the conditions investigated. The deposition of the capping phospholipid layer over the payload also favored the polymer relaxation contribution in the drug release, featuring new strategies to investigate the drug release in PEM.

Dataset Information

Imprinting of metal receptors into multilayer polyelectrolyte films: fabrication and applications in marine antifouling.

Publications

Imprinting of metal receptors into multilayer polyelectrolyte films: fabrication and applications in marine antifouling.

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