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Biomedical subjects

Craig A Grimes

Publications and source records attributed to Craig A Grimes.

At least 19 recordsLinked to original sources

Anodic growth of highly ordered TiO2 nanotube arrays to 134 microm in length.

Described is the fabrication of self-aligned highly ordered TiO(2) nanotube arrays by potentiostatic anodization of Ti foil having lengths up to 134 mum, representing well over an order of magnitude increase in length thus far reported. We have achieved the very long nanotube arrays in fluoride ion containing baths in combination with a variety of nonaqueous organic polar electrolytes including dimethyl sulfoxide, formamide, ethylene glycol, and N-methylformamide. Depending on the anodization voltage, pore diameters of the resulting nanotube arrays range from 20 to 150 nm. Our longest nanotube arrays yield a roughness factor of 4750 and length-to-width (outer diameter) aspect ratio of approximately 835. The as-prepared nanotubes are amorphous but crystallize with annealing at elevated temperatures. In initial measurements, 45 mum long nanotube-array samples, 550 degrees C annealed, under UV illumination show a remarkable water photoelectrolysis photoconversion efficiency of 16.25%.

Electrodes↗

Use of highly-ordered TiO(2) nanotube arrays in dye-sensitized solar cells.

We describe the use of highly ordered transparent TiO(2) nanotube arrays in dye-sensitized solar cells (DSCs). Highly ordered nanotube arrays of 46-nm pore diameter, 17-nm wall thickness, and 360-nm length were grown perpendicular to a fluorine-doped tin oxide-coated glass substrate by anodic oxidation of a titanium thin film. After crystallization by an oxygen anneal, the nanotube arrays are treated with TiCl(4) to enhance the photogenerated current and then integrated into the DSC structure using a commercially available ruthenium-based dye. Although the negative electrode is only 360-nm-thick, under AM 1.5 illumination the generated photocurrent is 7.87 mA/cm(2), with a photocurrent efficiency of 2.9%. Voltage-decay measurements indicate that the highly ordered TiO(2) nanotube arrays, in comparison to nanoparticulate systems, have superior electron lifetimes and provide excellent pathways for electron percolation. Our results indicate that remarkable photoconversion efficiencies may be obtained, possibly to the ideal limit of approximately 31% for a single photosystem scheme, with an increase of the nanotube-array length to several micrometers.

Calorimetry, Differential Scanning↗

Effects of localised, low-voltage pulsed electric fields on the development and inhibition of Pseudomonas aeruginosa biofilms.

This work describes the use of low-voltage (0.5 - 5 V) pulsed electric fields to prevent Pseudomonas aeruginosa biofilm development. Interdigitated electrodes (IDEs) with 29-mum spacing between 22-mum-wide electrodes, were used as a platform where the effect of localised, high-strength electric fields could be tested. Alternating current, square-wave pulses were applied to the IDEs in 1 sec intervals. A two-level, three-variable factorial design experiment was used to detect the effects of applied voltage, frequency, and pulse duty ratio (i.e. percentage of pulsing time over one cycle) on the inhibition of biofilm formation. The observations indicated that a pulse configuration of 1% duty ratio, 5 V, and 200 Hz frequency reduced the area of the electrodes covered by biofilm by 50%. In general, the application of low-duty ratio pulses had a positive effect on preventing biofouling. Comparatively, frequency and applied voltage were observed to have less influence on biofouling.

Biofilms↗

A rapid highly-sensitive endotoxin detection system.

This paper presents a rapid, highly-sensitive, and low-cost method of endotoxin quantification based on the use of stress-responsive magnetoelastic sensors, that monitor the gel formation (viscosity change) of the Limulus Amoebocyte Lysate (LAL) assay in response to endotoxin. Ribbon-like magnetoelastic sensors, 12.7 mm x 6 mm x 28 microm, were immersed in a LAL assay after mixing with test samples of variable endotoxin concentration, and the decrease in resonance amplitude of the sensor was recorded as a function of time. Experimental results show excellent correlation between endotoxin concentration and the maximum clot rate, determined by taking the minimum point of the first derivative of the amplitude-time curve, as well as the clotting-time, defined as the time that corresponds to the maximum clot rate. Using a LAL gel-clot assay with a sensitivity of 0.06 EU/ml (EU: endotoxin unit), the magnetoelastic sensor based technology can detect the presence of endotoxin at 0.0105 EU/ml in test requiring approximately 20 min. Unlike optical methods used for determining endotoxin concentration, the color of the test solution does not impact the magnetoelastic sensor measurement. Due to the small size of the sensor reader electronics and low cost, the magnetoelastic sensor based endotoxin detection system is ideally suited for wide-spread use in endotoxin screening for sepsis prevention.

Biosensing Techniques↗

Fabrication of highly ordered TiO2 nanotube arrays using an organic electrolyte.

Anodization of titanium in a fluorinated dimethyl sulfoxide (DMSO) and ethanol mixture electrolyte is investigated. The prepared anodic film has a highly ordered nanotube-array surface architecture. Using a 20 V anodization potential (vs Pt) nanotube arrays having an inner diameter of 60 nm and 40 nm wall thickness are formed. The overall length of the nanotube arrays is controlled by the duration of the anodization, with nanotubes appearing only after approximately 48 h; a 72 h anodization results in a nanotube array approximately 2.3 mum in length. The photoelectrochemical response of the nanotube-array photoelectrodes is studied using a 1 M KOH solution under both UV and visible (AM 1.5) illumination. Enhanced photocurrent density is observed for samples obtained in the organic electrolyte, with an UV photoconversion efficiency of 10.7%.

Journal Article↗

Fabrication and evaluation of nanoporous alumina membranes for osteoblast culture.

An understanding of osteoblast response to surface topography is essential for successful bone tissue engineering applications. Alumina has been extensively used as a substrate for bone tissue constructs. However, current techniques do not allow precise surface topography and orientation of the material. In this research, a two-step anodization process was optimized for the fabrication of nanoporous alumina membranes with uniform pore dimension and distribution. The anodization voltage can be varied to create nanoporous alumina membranes with pore sizes ranging from 30 to 80 nm in diameter. The impact of the nanoscale pores on osteoblast response was studied by evaluating cell adhesion, morphology, and matrix production. Scanning electron microscopy and atomic force microscopy were used to characterize the nanoporous alumina membranes. Osteoblast adhesion and morphology were investigated using scanning electron microscopy images and matrix production was characterized using energy dispersive spectroscopy. This research combined the advantages of using alumina, a material with proven biocompatibility and current orthopedic clinical applications, and incorporated porous features on the nanoscale which have been reported to improve osteoblast response.

Aluminum Oxide↗

Enhanced photocleavage of water using titania nanotube arrays.

In this study highly ordered titania nanotube arrays of variable wall thickness are used to photocleave water under ultraviolet irradiation. We demonstrate that the wall thickness and length of the nanotubes can be controlled via anodization bath temperature. We find that the nanotube wall thickness is a key parameter influencing the magnitude of the photoanodic response and the overall efficiency of the water-splitting reaction. For 22 nm inner pore diameter nanotube arrays, those fabricated in a 5 degrees C anodization bath, 224 nm length and 34 nm wall thickness produced a photoanodic response that was thrice that of a nanotube array fabricated in a 50 degrees C anodization bath, 120 nm length and 9 nm wall-thickness. At high anodic polarization, above 1 V, the quantum efficiency under 337 nm illumination was greater than 90%. For the 5 degrees C anodization bath samples (22 nm pore-diameter, 34 nm wall thickness), upon 320-400 nm illumination at an intensity of 100 mW/cm(2), hydrogen gas was generated at the power-time normalized rate of 960 micromol/h W (24 mL/h W) at an overall conversion efficiency of 6.8%. To the best of our knowledge, this hydrogen generation rate is the highest reported for a titania-based photoelectrochemical cell.

Journal Article↗

Attenuation of protein adsorption on static and oscillating magnetostrictive nanowires.

The research described here investigates the hypothesis that nanoarchitecture contained in a nanowire array is capable of attenuating the adverse host response generated when medical devices are implanted in the body. This adverse host response, or biofouling, generates an avascular fibrous mass transfer barrier between the device and the analyte of interest, disabling the implant if it is a sensor. Numerous studies have indicated that surface chemistry and architecture modulate the host response. These findings led us to hypothesize that nanostructured surfaces will inhibit the formation of an avascular fibrous capsule significantly. We are investigating whether arrays of oscillating magnetostrictive nanowires can prevent protein adsorption. Magnetostrictive nanowires were fabricated by electroplating a ferromagnetic metal alloy into the pores of a nanoporous alumina template. The ferromagnetic nanowires are made to oscillate by oscillating the magnetic field surrounding the wires. Radiolabeled bovine serum albumin, enzyme-linked immunosorbent assay (ELISA), and other protein assays were used to study protein adhesion on the nanowire arrays. These results display a reduced protein adsorption per surface area of static nanowires. Comparing the surfaces, 14-30% of the protein that absorbed on the flat surface adsorbed on the nanowires. Our contact angle measurements indicate that the attenuation of protein on the nanowire surface might be due to the increased hydrophilicity of the nanostructured surface compared to a flat surface of the same material. We oscillated the magnetostrictive wires by placing them in a 38 G 10 Hz oscillating magnetic field. The oscillating nanowires show a further reduction in protein adhesion where only 7-67% of the protein on the static wires was measured on the oscillating nanowires. By varying the viscosity of the fluid the nanowires are oscillated in, we determined that protein detachment is shear-stress modulated. We created a high shearing fluid with dextran, which reduced protein adsorption on the oscillating nanowires by 70% over nanowires oscillating in baseline viscosity fluid. Our preliminary studies strongly suggest that the architecture in the static nanowire arrays and the shear created by oscillating the nanowire arrays would attenuate the biofouling response in vivo.

Adsorption↗

Nanoporous alumina capsules for cellular macroencapsulation: transport and biocompatibility.

BACKGROUND: Currently, the most widely used treatment for diabetes is the daily subcutaneous injection of recombinant human insulin. Daily injections, however, cannot match the physiological biphasic behavior of normal insulin release, nor can they precisely meet the demands of food intake, exercise, and stress. Cellular encapsulation, or immunoisolation, is a possible solution to this problem. This cell-based therapy allows patients to receive the benefits of more physiological insulin and blood glucose regulation, without the need for immunosuppressants that are associated with organ or cell transplantation. METHODS: Immunoisolation capsules were fabricated out of aluminum and aluminum oxide using a two-step anodization procedure. The diffusion behavior of glucose, immunoglobulin G (IgG), and insulin were measured. Furthermore, the functionality and viability of encapsulated MIN6 cells were tested. Finally, live cells were stained and imaged using confocal microscopy. RESULTS: Data indicated that this device is effective in allowing the transport of relevant molecules such as glucose and insulin, while at the same time significantly impeding the transport of IgG, suggesting that it would be efficacious in protecting cell grafts in vivo. Furthermore, encapsulated cells were able to respond dynamically to glucose input signals. Finally, cell staining showed that the viability of encapsulated cells is maintained after 24 h, although the cells appear to be more heavily concentrated at the area that is closest to the membrane. CONCLUSIONS: This study has shown that nanoporous alumina membranes, with well-controlled pore sizes, can be used for the encapsulation of therapeutic cells and may provide an alternative encapsulation strategy for the treatment of diabetes.

Aluminum Oxide↗

Water-photolysis properties of micron-length highly-ordered titania nanotube-arrays.

We report the water photoelectrolysis and photoelectrochemical properties of the titania nanotube arrays as a function of nanotube crystallinity, length (up to 6.4 microm), and pore size. Most noteworthy of our results, under 320-400 nm illumination (98 mW/cm2) the titania nanotube-array photoanodes (area 1 cm2), pore size 110 nm, wall thickness 20 nm, and 6 microm length, generate hydrogen by water photoelectrolysis at a rate of 7.6 mL/hr, with a photoconversion efficiency of 12.25%. The energy-time normalized hydrogen evolution rate is 80 mL/hrW, the largest reported hydrogen photoelectrolysis generation rate for any material system by a factor of four. The highly-ordered nanotubular architecture appears to allow for superior charge separation and charge transport, with a calculated quantum efficiency of over 80% for incident photons with energies larger than the titania bandgap.

Electrochemistry↗

Numerical simulation of light propagation through highly-ordered titania nanotube arrays: dimension optimization for improved photoabsorption.

Propagation of electromagnetic waves in the ultraviolet-visible range (300 to 600 nm) through a unique highly-ordered titania nanotube array structure is studied using the computational technique of Finite Difference Time Domain (FDTD). Through numerical simulation the transmittance, reflectance and absorbance of the nanotube-arrays are obtained as a function of tube length and diameter. The nanotube-arrays are found to completely absorb light having wavelengths less than approximately 330 nm. For wavelengths above 380 nm absorption increases as a function of nanotube length, while above 435 nm absorption increases with decreasing pore size. Computational simulations closely match experimental measurements, indicating the suitability of the computational technique for guiding material optimization.

Absorption↗

Influence of nanoporous alumina membranes on long-term osteoblast response.

A major goal of bone tissue engineering is to design better scaffold configuration and materials to better control osteoblast behavior. Nanoporous architecture has been shown to significantly affect cellular response. In this work, nanoporous alumina membranes were fabricated by a two-step anodization method to investigate bone cell response. Osteoblasts were seeded on nanoporous alumina membranes to investigate both short-term adhesion and proliferation and long-term functionality and matrix production. Cell adhesion and proliferation were characterized using a standard MTT assay and cell counting. The total protein content was measured after cell lysis using the BCA assay. Matrix production was characterized in terms of surface concentrations of calcium and phosphorous, components of bone matrix, using X-ray photoelectron spectroscopy (XPS). The results from nanoporous alumina membranes were compared with those of amorphous alumina, aluminum, commercially available ANOPORE and glass. Results indicate improved osteoblast adhesion and proliferation and increased matrix production after 4 weeks of study.

Aluminum↗

A staphylococcal enterotoxin B magnetoelastic immunosensor.

A magnetoelastic immunosensor for detection of staphylococcal enterotoxin B (SEB) is described. The magnetoelastic sensor is a newly developed mass/elasticity-based transducer of high sensitivity having a material cost of approximately $0.001/sensor. Affinity-purified rabbit anti-SEB antibody was covalently immobilized on magnetoelastic sensors, of dimensions 6 mm x 2 mm x 28 microm. The affinity reaction of biotin-avidin and biocatalytic precipitation are used to amplify antigen-antibody binding events on the sensor surface. Horseradish peroxidase (HRP) and alkaline phosphatase were examined as the labeled enzymes to induce biocatalytic precipitation. The alkaline phosphatase substrate, 5-bromo-4-chloro-3-indolyl phosphate (BCIP) produces a dimer, which binds tightly to the sensor surface, inducing a change in sensor resonance frequency. The biosensor demonstrates a linear shift in resonance frequency with staphylococcal enterotoxin B concentration between 0.5 and 5 ng/ml, with a detection limit of 0.5 ng/ml.

Alkaline Phosphatase↗

Surface modification of nanoporous alumina surfaces with poly(ethylene glycol).

Nanoporous alumina surfaces have a variety of applications in biosensors, biofiltration, and targeted drug delivery. However, the fabrication route to create these nanopores in alumina results in surface defects in the crystal lattice. This results in inherent charge on the porous surface causing biofouling, that is, nonspecific adsorption of biomolecules. Poly(ethylene glycol) (PEG) is known to form biocompatible nonfouling films on silicon surfaces. However, its application to alumina surfaces is very limited and has not been well investigated. In this study, we have covalently attached PEG to nanoporous alumina surfaces to improve their nonfouling properties. A PEG-silane coupling technique was used to modify the surface. Different concentrations of PEG for different immobilization times were used to form PEG films of various grafting densities. X-ray photoelectron spectroscopy (XPS) was used to verify the presence of PEG moieties on the alumina surface. High-resolution C1s spectra show that with an increase in concentration and immobilization time, the grafting density of PEG also increases. Further, a standard overlayer model was used to calculate the thickness of PEG films formed using the XPS intensities of the Al2p peaks. The films formed by this technique are less than 2.5 nm thick, suggesting that such films will not clog the pores which are in the range of 70-80 nm.

Adsorption↗

A magnetoelastic bioaffinity-based sensor for avidin.

A magnetoelastic bioaffinity sensor coupled with biocatalytic precipitation is described for avidin detection. The non-specific adsorption characteristics of streptavidin on different functionalized sensor surfaces are examined. It is found that a biotinylated poly(ethylene glycol) (PEG) interface can effectively block non-specific adsorption of proteins. Coupled with the PEG immobilized sensor surface, alkaline phosphatase (AP) labeled streptavidin is used to track specific binding on the sensor. This mass-change-based signal is amplified by the accumulation on the sensor of insoluble products of 5-bromo-4-chloro-3-indolyl phosphate catalyzed by AP. The resulting mass loading on the sensor surface in turn shifts the resonance frequency of the magnetoelastic sensors, with an avidin detection limit of approximately 200 ng/ml.

Avidin↗

A wireless, remote query glucose biosensor based on a pH-sensitive polymer.

This paper describes a wireless, remote query glucose biosensor using a ribbonlike, mass-sensitive magnetoelastic sensor as the transducer. The glucose biosensor is fabricated by first coating the magnetoelastic sensor with a pH-sensitive polymer and upon it a layer of glucose oxidase (GOx). The pH-responsive polymer swells or shrinks, thereby changing mass, respectively, in response to increasing or decreasing pH values. The GOx-catalyzed oxidation of glucose produces gluconic acid, inducing the pH-responsive polymer to shrink, which in turn decreases the polymer mass. In response to a time-varying magnetic field, a magnetoelastic sensor mechanically vibrates at a characteristic resonance frequency, the value of which inversely depends on sensor mass loading. As the magnetoelastic films are magnetostrictive, the vibrations launch magnetic flux that can be remotely detected using a pickup coil. Hence, changes in the resonance frequency of a passive magnetoelastic transducer are detected on a remote query basis, without the use of physical connections to the sensors.The sensitivity of the glucose biosensors decreases with increasing ionic strength; at physiological salt concentrations, 0.6 mmol/L of glucose can be measured. At glucose concentrations of 1-10 mmol/L, the biosensor response is reversible and linear, with the detection limit of 0.6 mmol/L corresponding to an error in resonance frequency determination of 20 Hz. Since no physical connections between the sensor and the monitoring instrument are required, this sensor can potentially be applied to in vivo and in situ measurement of glucose concentrations.

Acrylates↗

A titania nanotube-array room-temperature sensor for selective detection of hydrogen at low concentrations.

A tremendous variation in electrical resistance, from the semiconductor to metallic range, has been observed in titania nanotube arrays at room temperature, approximately 25 degrees C, in the presence of < or = 1000 ppm hydrogen gas. The nanotube arrays are fabricated by anodizing titanium foil in an aqueous electrolyte solution containing hydrofluoric acid and acetic acid. Subsequently, the arrays are coated with a 10 nm layer of palladium by evaporation. Electrical contacts are made by sputtering a 2 mm diameter platinum disk atop the Pd-coated nanotube array. These sensors exhibit a resistance variation of the order of 10(4) in the presence of 100 ppm hydrogen at 25 degrees C. The sensors demonstrate complete reversibility, repeatability, high selectivity, negligible drift and wide dynamic range. The nanoscale geometry of the nanotubes, in particular the points of tube-to-tube contact, is believed to be responsible for the outstanding hydrogen gas sensitivities.

Acetic Acid↗

Synthesis and characterization of extremely uniform Fe-Co-Ni ternary alloy nanowire arrays.

We have fabricated extremely uniform arrays of polycrystalline Fe-Co-Ni ternary alloy nanowires having composition Fe 12.3 wt.%, Co 43.9 wt.% and Ni 43.8 wt.%. The wires are made by electrodeposition into nanoporous alumina templates, using an electrodeposition voltage of 15 V at 1000 Hz. Nanowires have been fabricated having diameters ranging from 43 nm to 120 nm, and lengths of 3 microm to 7 microm, as dependent upon template topology. The magnetization easy axis lies along the nanowire length, with an easy axis coercivity of 72 kA/m.

Alloys↗