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Advances in functional coatings and methods to deposit them are critical in enhancing the functionality and performance of 3D micro-architected devices in applications encompassing energy storage, electronics, as well as selective and high-capacity molecular adsorption. Electrodeposition as a non-line-of-sight fabrication method for thin films is readily adapted to modify micro 3D substrates with functional coatings. However, most polymer electrodeposition so far has been achieved by electrochemically initiated chain-growth polymerization which causes uncontrolled polymer formation when applied on 3D micro-architected substrate. Here, this project developed the electrodeposition of polymer thin films utilizing electrocoupling reaction between bromoisobutyrate (bib) and acrylate functionalities to form a step-growth polymer network. The influence of molecular concentration, solvents, and end-group ratio are investigated on planar gold electrodes, enabling tailorable control over the film thickness, molecular permeability, and chemical composition. The optimized method is applied to coat a layer with solid polymer electrolyte on a low-tortuosity 3D Carbon electrode with high aspect ratio pores of micron-scale diameters. As a result, the entire pore surface of the 3D carbon electrode is effectively enveloped by a sub-micron polymer film. The deposited polymer film exhibits high electronic resistance and can serve as a solid polymer electrolyte. This approach decouples the polymer functionality from its electrodeposition chemistry while preventing uncontrolled polymer formation away from the surface and can therefore be a universal method to coat various conductive micro-architected 3D substrates with tailorable functional polymers. / 2025-08-29T00:00:00Z

The behavior of miscible polymer mixtures at surfaces depends to a large extent on the thermodynamics of mixing in the bulk. The relative importance of bulk and surface interactions has been investigated for polymer blends and solutions using neutron reflection. Segregation in miscible blends of SAN copolymers is driven by surface tension differences between the two components, which arise from AN content differences. The extent of demixing at the surface is found to depend strongly on the Flory-Huggins interaction parameter, $\chi.$ For dilute solutions of terminally carboxylated polystyrenes in contact with an SiO$\sb2$ wall, polymer adsorption is dominated by the SiO$\sb2$/COOH interaction. Even under these "strong wall" conditions, the extent of adsorption is found to be sensitive to $\chi.$

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