Engineering Shelf-Stable Coating for Microfluidic Organ-on-a-Chip Using Bioinspired Catecholamine Polymers.

The conceptualization of body-on-a-chip in 2004 resulted in a new approach for studying human physiology in three-dimensional culture. Despite pioneering works and the progress made in replicating human physiology on-a-chip, the stability, reliability, and preservation of cell-culture-treated microfluidic chips remain a challenge. The development of a reliable surface treatment technique to more efficiently and reproducibly modify microfluidic channels would significantly simplify the process of creating and implementing organ-on-a-chip (OOC) systems. In this work, a new flow-based coating technique using bioinspired polymers was implemented to create reliable, reproducible, ready-to-use microfluidic cell culture chips for OOC studies. Single-channel polydimethylsiloxane microfluidic chips were coated with the bioinspired catecholamine polymers, polydopamine (PDA) and polynorepinephrine (PNE), using a flow-based coating technique. The functionality of the resulting microfluidic chips was evaluated by extensive surface characterizations, at 130 °C, in the presence of various cleaning and culture media in static and flow conditions regularly used in OOCs and tested for shelf life by storing the coated microfluidic chips for 4 months at room temperature. Microfluidic chips coated with polycatecholamine were then seeded with the mouse cancer cell line Cath.a.differentiated (CAD) and with the normal human cerebral microvascular endothelial cell line human cerebral microvascular endothelial cells (hCMEC)/D3. Cell viability, cell phenotype, and cell functionality were assessed to evaluate the performance of both the coatings and the surface treatment technique. Both PDA- and PNE-coated microfluidic chips maintained high viability, phenotype, and functionality of CAD cells and hCMEC/D3 cells. In addition, CAD cells retained high viability when they were cultured in both the polymer-coated chips, which were stored at room temperature for up to 120 days. These results suggest that flow-based techniques to coat surfaces with polycatecholamines can be used to generate ready-to-use microfluidic OOC chips that offer long-term stability and reliability for the culture of cell types with application in pathophysiological studies and drug screening.

Gold nanoparticle assembly on porous silicon by pulsed laser induced dewetting.

This work reports the influence of the substrate in the pulsed laser-induced dewetting (PLiD) of Au thin films for the fabrication of nanoparticle (NP) arrays. Two substrates were studied, i.e., polished silicon and porous silicon (PS), the latter being fabricated via electrochemical anodization in HF-containing electrolytes. The effect of both PLiD and substrate preparation parameters was explored systematically. On polished silicon substrates, it has been shown that uniform, randomly arranged NPs between 15 ± 7 nm and 89 ± 19 nm in diameter are produced, depending on initial thin film thickness. On PS however, there are topographical features that lead to the formation of ordered NPs with their diameters being controllable through laser irradiation time. The presence of surface pores and the appearance of surface ripples under low HF concentrations (<9.4 wt%) during electrochemical anodization results in this unique dewetting behaviour. Through AFM analysis, it has been determined that the ordered NPs sit within the valleys of the ripples, and form due to the atomic mobility enabled using the PLiD approach. This work has demonstrated that the utilization of topographically complex PS substrates results in size controllable and ordered NPs, while the use of polished Si does not enable such control over array fabrication.

Bioelectrochemical remediation of phenanthrene in a microbial fuel cell using an anaerobic consortium enriched from a hydrocarbon-contaminated site.

Polycyclic aromatic hydrocarbons (PAH) are organic pollutants that require remediation due to their detrimental impact on human and environmental health. In this study, we used a novel approach of sequestering a model PAH, phenanthrene, onto a solid carbon matrix bioanode in a microbial fuel cell (MFC) to assess its biodegradation coupled with power generation. Here, the bioanode serves as a site for enrichment of electroactive and hydrocarbon-degrading microorganisms, which can simultaneously act to biodegrade a pollutant and generate power. Carbon cloth electrodes loaded with two rates of phenanthrene (2 and 20 mg cm-2) were compared using dual chamber MFCs that were operated for 50 days. The lower loading rate of 2 mg cm-2 was most efficient in the degradation of phenanthrene and had higher power production capacities (37 mW m-2) as compared to the higher loading rate of 20 mg cm-2 (power production of 19.2 mW m-2). FTIR (Fourier-Transform Infrared Spectroscopy) analyses showed a depletion in absorbance peak signals associated with phenanthrene. Microbes known to have electroactive properties or phenanthrene biodegradation abilities like Pseudomonas, Rhodococcus, Thauera and Ralstonia were enriched over time in the MFCs, substantiating the electrochemical and FTIR analyses. The MFC approach taken here thus offers great promise towards PAH bioelectroremediation.

Polyethylenimine Modified Graphene-Oxide Electrochemical Immunosensor for the Detection of Glial Fibrillary Acidic Protein in Central Nervous System Injury.

Glial fibrillary acidic protein (GFAP) is as an intermediate filament protein expressed by certain cells in the central nervous system (CNS). GFAP has been recognized as a reliable biomarker of CNS injury. However, due to the absence of rapid and easy-to-use assays for the detection of CNS injury biomarkers, measuring GFAP levels to identify CNS injury has not attained widespread clinical implementation. In the present work, we developed a polyethylenimine (PEI) coated graphene screen-printed electrode and used it for highly sensitive immunosensing of GFAP. Covalent binding of GFAP antibody to the PEI-modified electrode surface along with electrochemical impedance spectroscopy was used for detecting the change in the electrical conductivity of the electrodes. A highly linear response was recorded for various GFAP concentrations. Quantitative, selective, and label-free detection was achieved in the dynamic range of 1 pg mL-1 to 100 ng mL-1 for GFAP spiked in phosphate buffer saline, artificial cerebrospinal fluid, and human blood serum. The performance of the immunosensor was further validated and correlated by testing samples with the commercially available enzyme-linked immunosorbent assay method. This functionalized electrode could be used clinically for rapid detection and monitoring of CNS injury.

Fluorescent polycatecholamine nanostructures as a versatile probe for multiphase systems.

Shape and size controlled nanostructures are critical for nanotechnology and have versatile applications in understanding interfacial phenomena of various multi-phase systems. Facile synthesis of fluorescent nanostructures remains a challenge from conventional precursors. In this study, bio-inspired catecholamines, dopamine (DA), epinephrine (EP) and levodopa (LDA), were used as precursors and fluorescent nanostructures were synthesized via a simple one pot method in a water-alcohol mixture under alkaline conditions. DA and EP formed fluorescent spheres and petal shaped structures respectively over a broad spectrum excitation wavelength, whereas LDA did not form any particular structure. However, the polyepinephrine (PEP) micropetals were formed by weaker interactions as compared to covalently linked polydopamine (PDA) nanospheres, as revealed by NMR studies. Application of these fluorescent structures was illustrated by their adsorption behavior at the oil/water interface using laser scanning confocal microscopy. Interestingly, PDA nanospheres showed complete coverage of the oil/water interface despite its hydrophilic nature, as compared to hydrophobic PEP micropetals which showed a transient coverage of the oil/water interface but mainly self-aggregated in the water phase. The reported unique fluorescent organic structures will play a key role in understanding various multi-phase systems used in aerospace, biomedical, electronics and energy applications.

A Modular Approach To Study Protein Adsorption on Surface Modified Hydroxyapatite.

Biocompatible inorganic nano- and microcarriers can be suitable candidates for protein delivery. This study demonstrates facile methods of functionalization by using nanoscale linker molecules to change the protein adsorption capacity of hydroxyapatite (HA) powder. The adsorption capacity of bovine serum albumin as a model protein has been studied with respect to the surface modifications. The selected linker molecules (lysine, arginine, and phosphoserine) can influence the adsorption capacity by changing the electrostatic nature of the HA surface. Qualitative and quantitative analyses of linker-molecule interactions with the HA surface have been performed by using NMR spectroscopy, zeta-potential measurements, X-ray photoelectron spectroscopy, and thermogravimetric analyses. Additionally, correlations to theoretical isotherm models have been calculated with respect to Langmuir and Freundlich isotherms. Lysine and arginine increased the protein adsorption, whereas phosphoserine reduced the protein adsorption. The results show that the adsorption capacity can be controlled with different functionalization, depending on the protein-carrier selections under consideration. The scientific knowledge acquired from this study can be applied in various biotechnological applications that involve biomolecule-inorganic material interfaces.