Intrinsic Elasticity of a Three-Dimensional Macroporous Scaffold Governs the Kinetics of In Situ Biomimetic Reactions

Porous materials that synergistically combine high reversible mechanical elasticity with tunable in situ reaction kinetics can find several biological and industrial applications. However, such materials remain elusive in the literature. Herein, we show that by utilizing the intrinsic elastic proper...

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Veröffentlicht in:Chemistry of materials 2022-11, Vol.34 (22), p.9892-9902
Hauptverfasser: Hegde, Lohitha R., Tikader, Baishakhi, Srivatsav, Aswin T., Kar, Sandip, Sharma, Kamendra P.
Format: Artikel
Sprache:eng
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Zusammenfassung:Porous materials that synergistically combine high reversible mechanical elasticity with tunable in situ reaction kinetics can find several biological and industrial applications. However, such materials remain elusive in the literature. Herein, we show that by utilizing the intrinsic elastic property of a 3D macroporous material/scaffold comprising polymer-coated biomimetic ceria nanoparticles, the rate of in situ dephosphorylation reactions can be enhanced efficiently. The elasticity of the scaffold is dynamically controlled by employing compression–decompression, [C–D], cycles. Varying the [C–D] frequency from 0 to 4 increases the formation of dephosphorylation reaction products, such as molecular p-nitrophenol or the in situ self-assembled Fmoc-l-tyrosine-based network. Further, we employ a numerical method improvised on an existing stochastic reaction diffusion approach to explain the unusual increase in product formation as a function of the frequency of the [C–D] cycles. The proposed computational methodology predicts rational design of the enzyme-mimicking material by analyzing the efficiency of the product formation under various absolute amounts of the catalyst and substrate levels, suggesting possible applications of such materials. Finally, as a proof of concept, we demonstrate the use of these materials for culturing mammalian cells, which suggests their potential biological applications after implementing appropriate post-synthetic chemical modifications.
ISSN:0897-4756
1520-5002
DOI:10.1021/acs.chemmater.2c01792