As nature's choice in designing complex architectures, the bottom-up assembly of nanoscale building blocks offers unique solutions in achieving more complex and smaller morphologies with wide-ranging applications in medicine, energy, and materials science as compared to top-down manufacturing. In this work, we employ charged tobacco mosaic virus (TMV-wt and TMV-lys) nanoparticles in constructing multilayered fibrous networks via electrostatic layer-by-layer (LbL) deposition. In neutral aqueous media, TMV-wt assumes an anionic surface charge. TMV-wt was paired with a genetically engineered TMV-lys variant that displays a corona of lysine side chains on its solvent-exposed surface. The electrostatic interaction between TMV-wt and TMV-lys nanoparticles became the driving force in the highly controlled buildup of the multilayer TMV constructs. Since the resulting morphology closely resembles the 3-dimensional fibrous network of an extracellular matrix (ECM), the capability of the TMV assemblies to support the adhesion of NIH-3T3 fibroblast cells was investigated, demonstrating potential utility in regenerative medicine. Lastly, the layer-by-layer deposition was extended to release the TMV scaffolds as free-standing biomembranes. To demonstrate potential application in drug delivery or vaccine technology, cargo-functionalized TMV biofilms were programmed.
A colloidal sphere-patterned polyterthiophene thin film sensor with high binding affinity and selectivity towards aspartame was fabricated using a technique combining molecular imprinting and colloidal sphere lithography (CSL). The successful imprinting of aspartame into electropolymerized molecularly imprinted polymer generated artificial recognition sites capable of rebinding aspartame into the microporous film, which was sensitively detected using quartz crystal microbalance measurements. The resulting sensor exhibited a good linear response after exposure to aspartame concentrations ranging from 12.5 μM to 200 μM and limit of detection of ~31 μM. It also demonstrated a high selectivity towards aspartame as compared to other peptidebased analogs including alanine-phenylalanine (Ala-Phe), alanine-glutamine (Ala-Gln), glycylglycine (Gly-Gly), and arginylglycylaspartic acid (RGD). The formation of the highly ordered micropatterned surface was induced and monitored in situ by electrochemical quartz crystal microbalance and atomic force microscopy. Analyte imprinting and removal were characterized using X-ray photoelectron spectroscopy. Based on molecular modeling (semiempirical AM1 quantum calculations), the formation of a stable pre-polymerization complex due to the strong hydrogen bonding interactions between the terthiophene monomer and aspartame played a key role in the effective aspartame imprinting and detection.
Nanostructured mesoscale materials find wide-ranging applications in medicine and energy. Top-down manufacturing schemes are limited by the smallest dimension accessible; therefore, we set out to study a bottom-up approach mimicking biological systems, which self-assemble into systems that orchestrate complex energy conversion functionalities. Inspired by nature, we turned toward protein-based nanoparticle structures formed by plant viruses, specifically the cowpea mosaic virus (CPMV). We report the formation of hierarchical CPMV nanoparticle assemblies on colloidal-patterned, conducting polymer arrays using a protocol combining colloidal lithography, electrochemical polymerization, and electrostatic adsorption. In this approach, a hexagonally close-packed array of polystyrene microspheres was assembled on a conductive electrode to function as the sacrificial colloidal template. A thin layer of conducting polypyrrole material was electrodeposited within the interstices of the colloidal microspheres and monitored in situ using electrochemical quartz crystal microbalance with dissipation (EC-QCM-D). Etching the template revealed an inverse opaline conducting polymer pattern capable of forming strong electrostatic interactions with CPMV and therefore enabling immobilization of CPMV on the surface. The CPMV-polymer films were characterized by atomic force microscopy (AFM) and X-ray photoelectron spectroscopy (XPS). Furthermore, molecular probe diffusion experiments revealed selective ion transport properties as a function of the presence of the CPMV nanoparticles on the surface. Lastly, by utilizing its electromechanical behavior, the polymer/protein membrane was electrochemically released as a free-standing film, which can potentially be used for developing high surface area cargo delivery systems, stimuli-responsive plasmonic devices, and chemical and biological sensors.
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