ArticleChemistry of materials : a publication of the American Chemical Society2025
Elucidating the Kinetics and Thermodynamics of Organic Vapor Phase Infiltration and Molecular Layer Deposition for Dissolution Resilient Polymers.
Article in Chemistry of materials : a publication of the American Chemical Society, 2025. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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Abstract
Vapor phase chemical synthesis techniques, such as atomic layer deposition (ALD) and vapor phase infiltration (VPI), enable molecular-level tailoring of polymeric materials through deposition or incorporation of inorganic components. However, benefits are often paired with compromised mechanical stability and organic-inorganic bonds that are prone to degradation via hydrolysis. To address these limitations, we investigate all-organic VPI and molecular layer deposition (MLD) chemistries as a strategy for enhancing polymer properties. We examine the reaction-diffusion kinetics and thermodynamic behavior of three aromatic step-growth polymerization reactions: polyamide (isophthaloyl chloride + m-phenylenediamine, MPD), polyurea (1,4-phenylene diisocyanate + MPD), and polyimine (terephthalaldehyde + MPD). Their material growth occurs via MLD at the surfaces of nonabsorbing silicon and zirconia. Organic VPI occurs within the bulk of nucleophile-rich polyvinyl alcohol (PVA), but not through physical entrapment in unreactive polystyrene and poly-(methyl methacrylate). Using a reaction-diffusion model, we quantify diffusion-limited polyamide and reaction-limited polyurea nucleation behavior in PVA, identifying key parameters: diffusivity, reaction rate, and Damköhler number. Unlike inorganic alumina treatment, organic modification enhances dissolution-resistance in PVA, preserving polymer integrity and resisting hydrolysis even in harsh pH 13 solutions. This study demonstrates the potential of all-organic material deposition for synthesizing novel polymers with improved durability and solvent resilience.
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