We report the assembly of metal-polyphenol complex (MPC) films and capsules through the sequential deposition of iron(III) ions (Fe(III)) and a natural polyphenol, tannic acid (TA), driven by metal–ligand coordination. Stable Fe(III)/TA films and capsules were formed, indicating lateral and longitudinal cross-linking of TA by Fe(III) in the film structure. Quartz crystal microbalance, ultraviolet–visible (UV-vis) spectrophotometry, and X-ray photoelectron spectroscopy were carried out to quantitatively analyze the film growth. A comparison of the MPC capsules prepared through multistep assembly with those obtained through one-step deposition, as reported previously [Ejima et al., Science 2013, 341, 154–156], reveals substantial differences in the nature of complexation and in their physicochemical properties, including permeability, stiffness, and degradability. This study highlights the importance of engineering MPC films with different properties through implementing different assembly methods.
A novel fabrication process is presented using monodisperse PMMA latex particles to facilitate controlled microvoid formation. This results in hierarchically rough surfaces exhibiting ∼90% optical transmission while retaining water contact angle (θ) of 170°. Synchrotron small angle X-ray scattering, AFM roughness measurements, and theoretical modeling suggests that a surface morphology with fractal dimension of ∼2.6 and R a < 400 nm allows for the optimum coupling of roughness-induced superhydrophobicity and optical transparency. Interestingly, surfaces of vastly different roughness (R rms) exhibited similar water contact angles, highlighting a limitation of traditional AFM roughness measurements in quantifying multiscale rough surfaces. An alternate method considering fractal dimension is presented as a more complete quantifier of hierarchical surface morphology in relation to surface wetting behavior.
Crosslinked polyelectrolyte multilayer membranes are synthesized with salt rejection values approaching those of commercial desalination membranes, but with increased chlorine resistance. The membranes are fabricated directly onto porous commercial substrates. Subsequent crosslinking of the polycation layers with glutaraldehyde leads to NaCl rejections of up to 97%, while the incorporation of a highly sulfonated polysulfone polyanion leads to high chlorine resistance.
We report engineered hydrogel thin-films with varying degrees of covalent crosslinking, which demonstrate enhanced HeLa cell adhesion with decreasing film stiffness. This trend is contrary to previous findings for tumour cell adhesion on hydrogel substrates, and is attributed to the extremely soft nature of the films studied, allowing for a greater cell/film contact area and the development of adhesive focal contacts. Adhesion based on mechanical tuning of the film was decoupled from chemical effects through characterisation and analysis of film surface roughness, hydrophobicity and charge. Control over cellular adhesion, differentiation, migration and recolonisation through substrate modification has recently emerged as a topic of considerable research effort. 1-5 Understanding these interactions allows for regulation of stem-cell 65
Surfaces consisting of sub micron holes (0.420-0.765 μm) engineered into nanoparticle (12 nm) coatings were examined for marine antifouling behaviour that defines early stage settlement. Immersed surfaces were found to be resistant to a 5-hour attachment assay of Amphora coffeaeformis, a marine organism commonly found in abundance on fouled substrates such as foul-releasing paints and self-polishing coatings. Attachment inhibition was attributed to the accessibility of diatoms to the surface. This was governed by the size and morphology of trapped interfacial air pockets measured in-situ using synchrotron small angle x-ray scattering. Surfaces containing larger pores (0.765 μm) exhibited the highest resistance. Macroscopic wettability via contact angle measurements however remained at 160° and sliding angle of < 5° and was found to be independent of pore size and not indicative of early stage fouling behaviour. The balance of hierarchical nano/micro length scales was critical in defining the early stage stability of biofouling character of the interface.
Carbonic anhydrase (CA) is a native enzyme that facilitates the hydration of carbon dioxide into bicarbonate ions. This study reports the fabrication of thin films of active CA enzyme onto a porous membrane substrate using layer-by-layer (LbL) assembly. Deposition of multilayer films consisting of polyelectrolytes and CA was monitored by quartz crystal microgravimetry, while the enzymatic activity was assayed according to the rates of p-nitrophenylacetate (p-NPA) hydrolysis and CO2 hydration. The fabrication of the films onto a nonporous glass substrate showed CO2 hydration rates of 0.52 ± 0.09 μmol cm(-2) min(-1) per layer of bovine CA and 2.6 ± 0.7 μmol cm(-2) min(-1) per layer of a thermostable microbial CA. The fabrication of a multilayer film containing the microbial CA on a porous polypropylene membrane increased the hydration rate to 5.3 ± 0.8 μmol cm(-2) min(-1) per layer of microbial CA. The addition of mesoporous silica nanoparticles as a film layer prior to enzyme adsorption was found to increase the activity on the polypropylene membranes even further to a rate of 19 ± 4 μmol cm(-2) min(-1) per layer of microbial CA. The LbL treatment of these membranes increased the mass transfer resistance of the membrane but decreased the likelihood of membrane pore wetting. These results have potential application in the absorption of carbon dioxide from combustion flue gases into aqueous solvents using gas-liquid membrane contactors.
Metal-phenolic network (MPN) coatings have generated increasing interest owing to their biologically inspired nature, facile fabrication, and near-universal adherence, especially for biomedical applications. However, a key issue in biomedicine is protein fouling, and the adsorption of proteins on tannic acid-based MPNs remains to be comprehensively studied. Herein, we investigate the interaction of specific biomedically relevant proteins in solution (bovine serum albumin (BSA), immunoglobulin G (IgG), fibrinogen) and complex biological media (serum) using layer-by-layer-assembled tannic acid/Fe III MPN films. When Fe III was the outermost layer, galloyl-modified poly(2-ethyl-2-oxazoline) (P(EtOx)-Gal) could be grafted to the films through coordination bonds. Protein fouling and bacterial adhesion were greatly suppressed after functionalization with P(EtOx)-Gal and the mass of adsorbed protein was reduced by 44-92%. Interestingly, larger proteins adsorbed more on both the MPNs and P(EtOx)-functionalized MPNs. This study provides fundamental information on the interactions of MPNs with single proteins, mixtures of proteins as encountered in serum, and the noncovalent, coordination-based, functionalization of MPN films.
The current study reports the fabrication and characterization of superhydrophobic surfaces with increasing nanoroughness by decreasing silica nanoparticle size in a sol–gel matrix. Using small-angle X-ray scattering (SAXS) measurements allowed for the direct quantification of air entrapped at the interface, revealing for the first time that significant air remains on hierarchical surfaces despite observed droplet pinning through hysteresis measurements. Combining contact angle hysteresis and SAXS measurements of the surfaces immersed in sodium dodecylsulfate (SDS) solutions with Cassie and Tadmor’s model, a series of predicted contact angles were generated, comparing wetting transition mechanisms based on wetting line advance, droplet adhesion/pinning, and interfacial air entrapment. The study provided confirmation of key theoretical assumptions on wetting of hierarchical surfaces: (i) Cassie wetting of the nanofeatures is the preferred wetting progression on hierarchical surfaces; and (ii) the presence of an intermediate petal state is dependent on the level of nanoroughness as compared to the microroughness.
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