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Antimicrobial coatings in which the active agent (e.g. N-halamine) can regenerate activity represent a promising way to prevent microbial cross-contamination. A reported method for applying coatings containing antimicrobial N-halamines is layer-by-layer (LbL) application of polyelectrolytes, which form N-halamines upon cross-linking. Prior reports on dip layer-by-layer (LbL) fabrication have demonstrated the potential of this coating technology; however, spray LbL fabrication would enable more rapid coating and represents a more commercially translatable application technique. In this work, dip and spray LbL methods were used to coat polypropylene (PP) with N-halamine containing bilayers consisting of cross-linked polyethylenimine (PEI) and poly(acrylic acid) (PAA). Further experimentation with spray LbL fabrication used naturally occurring polyelectrolytes, chitosan and alginate. Materials were characterized using atomic force microscopy (AFM), ellipsometry, contact angle, fourier transform infrared spectroscopy, a chlorine content assay, and a dye assay for amine quantification. All methods of coating application exhibited a 99.999% (5-log) reduction against Listeria monocytogenes with application time for spray LbL taking less than 10% of the time required for dip LbL. Spray LbL fabrication of N-halamines is a rapid and inexpensive method to fabricate rechargeable antimicrobial surfaces.

Layer-by-layer (LBL) polyelectrolyte capsules can be modified to incorporate stimuli such as superparamagnetic nanoparticles which respond to a magnetic field only when it is turned on. Thus, they can act as a switch to load or unload their drug cargo on demand. Specifically, magnetite is incorporated into bilayer capsules made of alternating poly(allylamine hydrochloride) (PAH) and poly(sodium-p-styrenesulfonate) (PSS) which surrounds calcium carbonate core. The core is then dissolved using ethylenediaminetetraacetic acid (EDTA). These capsules are loaded with at FITC-BSA conjugate and examined with fluorescence to show the unloading of the FITC-BSA from capsules as it brightens the entire field of view of the microscope. The results suggest that we can next load and unload an anticancer drug such as doxorubicin using the combination of microcapsule and alternating magnetic field (AMF) to treat the cancer cells. Preliminary data interprets that the low frequency AMF we use has little to no adverse effect cells viability. This coincides with the general thought that low frequency AMF signals are not harmful to humans. Therefore, as an alternative to hyperthermia methods which use heat, it may be possible to deliver the anticancer drugs specifically to the cells when and where it is needed.

This thesis presents work done to improve the switching speed and contrast performance of electrochromic devices. Layer-by-Layer (LbL) assembly was used to deposit thin electrochromic films of materials ranging from organic, inorganic, conducting polymers, etc. The focus was on developing new materials with high contrast and long lifecycles. A detailed switching-speed study of solid-state EC devices of already-developed (PEDOT (Poly(3,4-ethylenedioxythiophene)), polyviologen, inorganic) materials and some new materials (Prodot-Sultone) was performed. Work was done to achieve the optimum thickness and number of bilayers in LbL films resulting in high-contrast and fast switching. Device sizes were varied for comparison of the performance of the lab-made prototype device with the commercially available "small pixel" size displays. Symmetrical EC devices were fabricated and tested whenever conducting polymers are used as an EC material. This symmetrical configuration utilizes conducting polymers as an electroactive layer on each of two ITO-coated substrates; potential is applied to the two layers of similar conducting polymers and the device changes color from one redox state to another. This method, along with LbL film assembly, are the main factors in the improvement of switching speed results over already-published work in the literature. PEDOT results show that EC devices fabricated by LbL assembly with a switching speed of less than 30 ms make EC flat-panel displays possible by adjusting film thickness, device size, and type of material. The high contrast value (84%) for RuP suggests that its LbL films can be used for low-power consumption displays where contrast, not fastest switching, is the prime importance. In addition to the electrochromic work, this thesis also includes a section on the application of LbL assembly in fabricating electromechanical bending actuators. For bending actuators based on ionic polymer metal composites (IPMCs), a new class of conductive composite network (CNC) electrode was investigated, based on LbL self-assembled multilayers of conductive gold (Au) nanoparticles. The CNC of an electromechanical actuator fabricated with 100 bilayers of polyallylamine hydrochloride (PAH)/Au NPs exhibits high strain value of 6.8% with an actuation speed of 0.18 seconds for a 26 µm thick IPMC with 0.4 µm thick LbL CNCs under 4 volts. / Ph. D.

The formation of layered nanoparticle films on the surface of wood fibers is reported in this study. The layer-by-layer (LbL) assembly technique was comprehensively investigated as a non-covalent surface modification method for lignocellulosic fiber. Nanocomposite-based lignocellulosic fibers were successfully fabricated by sequential adsorption of oppositely charged poly(diallydimethylammonium) chloride (PDDA) and clay nanoparticles in a number of repeated deposition cycles. Nanocomposite fibers displayed layered structure as indicated by the electrokinetic potential studies and scanning electron microscopy (SEM) analysis. Layer-by-layer films of PDDA and clay impacted the thermal stability of wood fibers. Average degradation temperature at 5 and 10% weight loss for modified fibers with 4 bi-layers increased by up to ~24 and ~15°C, respectively. Significant char residue formed for the LbL modified fibers after heating to 800°C, indicating that the clay-based coating may serve as a barrier, creating an insulating layer to prevent further decomposition of the material. Layer-by-layer film formation on wood fibers was investigated as a function of parameters related to fiber composition and solution conditions (ie. presence of lignin, salt concentration and pH). Elemental analysis of modified fibers revealed that PDDA adsorption to the fibers was reduced for all solution conditions for the samples with the highest content of lignin. Upon extracting the non-covalently attached lignin, the samples showed the greatest amount of PDDA adsorption, reaching to 1.5% of total mass, under neutral solution conditions without the presence of added electrolyte. Furthermore, the influence of both the amount of PDDA adsorbed onto the fiber surface and electrokinetic potential of modified fibers on subsequent multilayer formation was quantified. Under select fiber treatments, great amount of PDDA/clay (up to ~75% total mass for only 4 bi-layers) was adsorbed onto wood fibers through the LbL process, giving these high surface area fibers nanocomposite coatings. LbL modified fibers were melt compounded with isotactic polypropylene (PP) and compression molded into test specimens. The effect of LbL modification as a function of the number of bi-layers on composite performance was tested using the tensile, flexural, dynamic mechanical and thermal properties of fiber reinforced thermoplastic composites. LbL modified fiber composites had similar modulus values but significantly lower strength values than those of unmodified fiber composites. However, composites composed of LbL modified fibers displayed increased elongation at break, increasing by more than 50%, to those of unmodified samples. DSC results indicated that crystallization behavior of PP is promoted in the presence of wood fibers. Both unmodified and LbL modified fibers are able to acts as nucleating agents, which cause an increase of the crystallinity of PP. Moreover, results from tensile and flexural strength, dynamic mechanical analysis and water absorption tests revealed that the material (PDDA or clay) at the terminal (outer) layer of LbL modified fiber influences the performance of the composites. These findings demonstrate control over the deposition of nanoparticles onto lignocellulosic fibers influencing terminal surface chemistry of the fiber. Further investigation into using renewable fibers as carriers of nanoparticle films to improve fiber durability, compounding with thermoplastics that have higher melt processing temperatures, and tailoring terminal surface chemistry to enhance adhesion is justified by this research. / Ph. D.