ORCID Profile
0000-0002-7048-1175
Current Organisation
University of South Australia
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Publisher: Elsevier BV
Date: 05-2018
DOI: 10.1016/J.IJPHARM.2018.04.003
Abstract: This study aimed to develop dry powder particles with surfaces enriched in hydrophobic material by manipulation of spray-drying conditions and to investigate the effect of hydrophobic surface enrichment on aerosolization of hygroscopic drug. The composite dry powder formulations of kanamycin (hygroscopic drug) and rif icin (hydrophobic drug) were produced by systematically (2
Publisher: Elsevier BV
Date: 2010
Publisher: Springer Science and Business Media LLC
Date: 02-06-2016
Publisher: MDPI AG
Date: 10-12-2012
DOI: 10.3390/MIN2040493
Publisher: Wiley
Date: 16-02-2008
Publisher: Elsevier BV
Date: 08-2020
Publisher: Elsevier BV
Date: 07-2011
DOI: 10.1016/J.IJPHARM.2011.04.014
Abstract: The objective of this study was to investigate if the coating extent created by a mechanofusion process corresponded with observed changes in bulk powder properties. A fine lactose powder (approximate median diameter 20 μm) was dry coated with magnesium stearate using from 0.1 to 5% (w/w) content. An ultra-thin coating layer of magnesium stearate was anticipated, but previous attempts to determine such thin layers on these fine particles have had limited success, with poor resolution. In this study, the surface coating was examined using the state-of-the-art XPS and ToF-SIMS systems. The powder flow was characterized by Carr index and shear cell testing. XPS was successfully applied to demonstrate variations in surface coverage, as a function of additive levels, and indicated near complete coating coverage at additive levels of 1% (w/w) and above. ToF-SIMS results supported such coating coverage assessment, and indicated coating uniformly across the fine particle surfaces. The flow metrics employed could then be related to the coating coverage metrics. The mechanofusion process also modified the apparent surface roughness observed by SEM and BET. It was suggested that the changes in the surface chemical composition exerted a more evident and direct impact on the powder cohesion and flow characteristics than the changes in the surface morphological properties after the mechanofusion in this study.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5TB00790A
Abstract: ToF-SIMS was successfully applied to characterize and quantify the EGF grafted on hollow mesoporous silica nanoparticles.
Publisher: Elsevier BV
Date: 03-2013
DOI: 10.1016/J.COLSURFB.2012.10.039
Abstract: The surface immobilization of proteins is an emerging field with applications in a wide range of important areas: biomedical devices, disease diagnosis, biosensing, food processing, biofouling, and bioreactors. Proteins, in Nature, often work synergistically, as in the important enzyme mixture, cellulase. It is necessary to preserve these synergies when utilizing surface immobilized proteins. However, the competitive displacement of earlier adsorbed proteins by other proteins with stronger binding affinities (the "Vroman effect") results in undesired layer instabilities that are difficult to control. Although this nanoscale phenomenon has been extensively studied over the last 40 years, the process through which this competitive exchange occurs is not well understood. This paper uses atomic force microscopy, QCM-D, TOF-SIMS, and in-solution TOF-MS to show that this competitive exchange process can occur through the turning of multilayer protein aggregates. This dynamic process is consistent with earlier postulated "transient complex" models, in which the exchange occurs in three stages: an initial layer adsorbs, another protein layer then embeds itself into the initial layer, forming a "transient complex " the complex "turns," exposing the first layer to solution proteins from the first layer desorb resulting in a final adsorbed protein composition that is enriched in proteins from the second layer.
Publisher: Informa UK Limited
Date: 16-04-2015
DOI: 10.3109/03639045.2014.908901
Abstract: Intensive dry powder coating (mechanofusion) with tablet lubricants has previously been shown to give substantial powder flow improvement. This study explores whether the mechanofusion of magnesium stearate (MgSt), on a fine drug powder can substantially improve flow, without preventing the powder from being directly compacted into tablets. A fine ibuprofen powder, which is both cohesive and possesses a low-melting point, was dry coated via mechanofusion with between 0.1% and 5% (w/w) MgSt. Traditional low-shear blending was also employed as a comparison. No significant difference in particle size or shape was measured following mechanofusion. For the low-shear blended powders, only marginal improvement in flowability was obtained. However, after mechanofusion, substantial improvements in the flow properties were demonstrated. Both XPS and ToF-SIMS demonstrated high degrees of a nano-scale coating coverage of MgSt on the particle surfaces from optimized mechanofusion. The study showed that robust tablets were produced from the selected mechanofused powders, at high-dose concentration and tablet tensile strength was further optimized via addition of a Polyvinylpyrrolidone (PVP) binder (10% w/w). The tablets with the mechanofused powder (with or without PVP) also exhibited significantly lower ejection stress than those made of the raw powder, demonstrating good lubrication. Surprisingly, the release rate of drug from the tablets made with the mechanofused powder was not retarded. This is the first study to demonstrate such a single-step dry coating of model drug with MgSt, with promising flow improvement, flow-aid and lubrication effects, tabletability and also non-inhibited dissolution rate.
Publisher: American Chemical Society (ACS)
Date: 08-06-2010
DOI: 10.1021/LA101253G
Abstract: We demonstrate the application of time-of-flight secondary ion mass spectrometry (TOF-SIMS) in conjunction with multivariate statistics to differentiate trace levels of denatured proteins in adsorbed monolayers specifically, human serum albumin (HSA) on oxidized silicon substrates. Subtle differences in protein conformation due to thermal denaturation of HSA, unable to be determined by dynamic light scattering nor circular dichroism, were differentiated by TOF-SIMS. The fragmentation pattern is highly sensitive to protein conformation, allowing assessment of relative amounts of proteins in mixtures and quantifying amounts of denatured protein in a s le. Discussion is presented on ascribing orientation and conformational differences between s les based upon TOF-SIMS spectra. This has implications for detecting denatured protein in biotechnology and medical applications.
Publisher: Elsevier BV
Date: 10-2015
DOI: 10.1016/J.EJPS.2015.07.016
Abstract: This study investigates the effects of a variety of coating materials on the flowability and dissolution of dry-coated cohesive ibuprofen powders, with the ultimate aim to use these in oral dosage forms. A mechanofusion approach was employed to apply a 1% (w/w) dry coating onto ibuprofen powder with coating materials including magnesium stearate (MgSt), L-leucine, sodium stearyl fumarate (SSF) and silica-R972. No significant difference in particle size or shape was measured following mechanofusion with any material. Powder flow behaviours characterised by the Freeman FT4 system indicated coatings of MgSt, L-leucine and silica-R972 produced a notable surface modification and substantially improved flow compared to the unprocessed and SSF-mechanofused powders. ToF-SIMS provided a qualitative measure of coating extent, and indicated a near-complete layer on the drug particle surface after dry coating with MgSt or silica-R972. Of particular note, the dissolution rates of all mechanofused powders were enhanced even with a coating of a highly hydrophobic material such as magnesium stearate. This surprising increase in dissolution rate of the mechanofused powders was attributed to the lower cohesion and the reduced agglomeration after mechanical coating.
Publisher: Elsevier BV
Date: 12-2015
DOI: 10.1016/J.WATRES.2015.09.031
Abstract: Time-of-Flight Secondary Ion Mass Spectrometry (ToF-SIMS) surface analysis was conducted to characterise deposits in polyethylene pipes used in a novel pilot water distribution system (PDS). The system consisted of four (4) parallel distribution systems receiving water from different treatment processes, ranging from conventional coagulation through to an advanced membrane filtration system. After two years of operation, the distribution system was shut down and s les of pipe were collected for autopsy analysis. Inlet and outlet s les from each PDS were collected for purpose of comparison. ToF-SIMS was used to assess chemical differences in surface biofilm accumulation and particulate deposition, which resulted as a consequence of the treatment method and operational mode of each system. These data supplemented previously collected bacteriological and chemical water quality data. Results from the inorganic analysis of the pipes were consistent with corrosion and contamination events that occurred upstream in the corresponding treatment systems. Principal component analysis of data on organic constituents showed oxygen and nitrogen containing fragments were associated with the treatment inlet and outlet s les. These types of signals can often be ascribed to biofilm polysaccharides and proteins. A trend was observed when comparing s les from the same PDS, showing an association of lower molecular weight (MW) organic fragments with the inlet and higher MW organic fragments with the outlet s les.
Publisher: Elsevier BV
Date: 09-2018
Publisher: Elsevier BV
Date: 08-2015
DOI: 10.1016/J.EJPB.2015.04.035
Abstract: The amino acid L-leucine has been demonstrated to act as a lubricant and improve the dispersibility of otherwise cohesive fine particles. It was hypothesized that optimum surface L-leucine concentration is necessary to achieve optimal surface and bulk powder properties. Polyvinylpyrrolidone was spray dried with different concentration of L-leucine and the change in surface composition of the formulations was determined using X-ray photoelectron spectroscopy (XPS) and time of flight-secondary ion mass spectrometry (ToF-SIMS). The formulations were also subjected to powder X-ray diffraction analysis in order to understand the relationship between surface concentration and solid-state properties of L-leucine. In addition, the morphology, surface energy and bulk cohesion of spray dried formulations were also assessed to understand the relation between surface L-leucine concentration and surface and bulk properties. The surface concentration of L-leucine increased with higher feed concentrations and plateaued at about 10% L-leucine. Higher surface L-leucine concentration also resulted in the formation of larger L-leucine crystals and not much change in crystal size was noted above 10% L-leucine. A change in surface morphology of particles from spherical to increasingly corrugated was also observed with increasing surface l-leucine concentration. Specific collapsed/folded over particles were only seen in formulations with 10% or higher l-leucine feed concentration suggesting a change in particle surface formation process. In addition, bulk cohesion also reduced and approached a minimum with 10% L-leucine concentration. Thus, the surface concentration of L-leucine governs particle formation and optimum surface L-leucine concentration results in optimum surface and bulk powder properties.
Publisher: Springer Science and Business Media LLC
Date: 16-10-2013
Publisher: The Electrochemical Society
Date: 2012
DOI: 10.1149/2.080202JES
Publisher: The Electrochemical Society
Date: 2014
DOI: 10.1149/2.053403JES
Publisher: Elsevier BV
Date: 10-2017
DOI: 10.1016/J.EJPB.2017.06.023
Abstract: Inhalable particles containing amorphous form of drugs or excipients may absorb atmospheric moisture, causing powder aggregation and recrystallization, adversely affecting powder dispersion and lung deposition. The present study aims to explore hydrophobic amino acids for protection against moisture in spray-dried amorphous powders, using disodium cromoglycate (DSCG) as a model drug. DSCG powders were produced by co-spray drying with isoleucine (Ile), valine (Val) and methionine (Met) in various concentrations (10, 20 and 40%w/w). Particle size distribution and morphology were measured by laser diffraction and scanning electron microscopy (SEM). Physiochemical properties of the powders were characterized by X-ray powder diffraction (XRPD), differential scanning calorimetry (DSC), thermogravimetric analysis (TGA) and dynamic vapor sorption (DVS). Particle surface chemistry was analyzed by X-ray photoelectron spectroscopy (XPS) and time-of-flight secondary ion mass spectrometry (ToF-SIMS). In vitro aerosolization performance was evaluated by a next generation impactor (NGI) after the powders were stored at 60% or 75% relative humidity (RH) for one month and three months. Ile, Val and Met significantly reduced the deleterious effect of moisture on aerosol performance, depending on the amount of amino acids in the formulation. Formulations containing 10% or 20% of Ile, Val and Met showed notable deterioration in aerosol performance, with fine particle fraction (FPF) reduced by 6-15% after one-month storage at both 60% and 75% RH. However, 40% Ile was able to maintain the aerosol performance of DSCG stored at 75% RH for one month, while the FPF dropped by 7.5% after three months of storage. In contrast, 40% Val or Met were able to maintain the aerosol performance at 60% RH storage but not at 75% RH. At 40%w/w ratio, these formulations had particle surface coverage of 94.5% (molar percent) of Ile, 87.1% of Val and 84.6% of Met, respectively, which may explain their moisture protection effects. Ile, Val and Met showed promising moisture protection effect on aerosol performance. The results broaden the understanding on the use of hydrophobic amino acids as an excipient for long-term storage of inhalation powders formulations that are hygroscopic.
Publisher: Elsevier BV
Date: 04-2018
DOI: 10.1016/J.IJPHARM.2018.02.026
Abstract: High dose delivery of drugs to the lung using a dry powder inhaler (DPI) is an emerging approach to combat drug-resistant local infections. To achieve this, highly aerosolizable powders are required. We hypothesized that co-spray-drying kanamycin, a hydrophilic hygroscopic antibiotic, with rif icin, a hydrophobic antibiotic, would produce inhalable particles with surfaces enriched in rif icin. Such particles would have higher aerosolization than kanamycin alone, and minimise the mass of powder for inhalation avoiding use of non-active excipients. Kanamycin was co-spray-dried with rif icin using a Buchi Mini Spray-dryer. All powders were inhalable in size (1.1-5.9 µm) and noncrystalline. X-ray photoelectron spectroscopy (XPS) and time-of-flight secondary ion mass spectrometry (ToF-SIMS) showed the surface of the combination powder was enriched with rif icin. In vitro aerosolization (fine particle fraction) determined by next generation impactor (NGI), dramatically improved from 29.5 ± 0.2% (kanamycin-only) to 78.2 ± 1.3% (kanamycin-rif icin combination). The combination powder was flake-shaped in morphology, stable at 15% and 53% RH and 25 ± 2 °C during one-month storage in an open Petri dish, and non-toxic (up to 50 µg/mL) to human alveolar and bronchial cell-lines. Surface enrichment of kanamycin by hydrophobic rif icin improves aerosolization, which may help to combat drug-resistant local infections by facilitating high dose delivery to deep lung.
Publisher: Springer Science and Business Media LLC
Date: 24-11-2015
Publisher: Elsevier BV
Date: 12-2012
DOI: 10.1016/J.ACTBIO.2012.07.029
Abstract: Antimicrobial peptides (AMPs) are promising alternatives to current treatments for bacterial infections. However, our understanding of the structural-functional relationship of tethered AMPs still requires further investigation to establish a general approach for obtaining consistent antimicrobial surfaces. In this study, we have systematically examined the effects of surface orientation of a broad-spectrum synthetic cationic peptide, melimine, on its antibacterial activity against Gram-positive and Gram-negative bacteria. The attachment of melimine to maleimide-functionalized glass was facilitated by addition of a single cysteine amino acid into the peptide sequence at the N-terminus (CysN) or C-terminus (CysC), or at position 13 (Cys13, approximately central). The successful attachment of the modified melimine was monitored using X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry (ToF-SIMS) with principle component analysis. The ToF-SIMS analysis clearly demonstrated structural difference between the three orientations. The peptide density for the modified surfaces was found to be between 3.5-4.0×10(-9)molcm(-2) using a modified Bradford assay. The ability of the surfaces to resist Pseudomonas aeruginosa and Staphylococcus aureus colonization was compared using fluorescence confocal microscopy. Reductions in total P. aeruginosa and S. aureus adhesion of 70% (p<0.001) and 83% (p<0.001), respectively, after 48h were observed for the melimine s les when compared to the blank control. We found that melimine attached via the N-terminus was the most effective in reducing total bacterial adhesion and bacterial viability with two- and four times (p<0.001) more activity than melimine attached via the C-terminus for P. aeruginosa and S. aureus, respectively. Furthermore, for Cys13, despite having the highest measured peptide density of the three surfaces, the higher concentration did not confer the greatest antibacterial effect. This highlights the importance of orientation of the peptides on the surface to efficacy. Our results suggest that the optimal orientation of the cationic residues is essential for maximum surface activity, whereby the optimal activity is obtained when the cationic portion is more available to interact with colonizing bacteria.
Publisher: American Chemical Society (ACS)
Date: 26-06-2014
DOI: 10.1021/AM501390V
Abstract: A robust and flexible approach is described for the straightforward preparation of multicellular tumor spheroids of controllable dimensions. The approach is based on a one-step plasma polymerization of the monomer allylamine carried out through conformal micropatterning physical masks that is used to deposit amine-rich (PolyAA) micrometer-scale features that promote cellular attachment and initiate the formation of multicellular spheroids. A simple backfilling step of the nonpolymerized poly(dimethylsiloxane) background with Pluronic F127 significantly reduced background cellular adhesion on the untreated substrate and, in turn, improved the quality of the spheroid formed. Tumor cells grown on the PolyAA/F127 patterned surfaces reliably formed multicellular spheroids within 24-48 h depending on the cell type. The dimension of the spheroids could be readily controlled by the dimension of the amine-rich micropatterns. This simple approach is compatible with the long-term culture of multicellular spheroids and their characterization with high-resolution optical microscopy. These features facilitate the development of on-chip assays, as demonstrated here for the study of the binding of transferrin-functionalized gold nanoparticles to multicellular tumor spheroids.
Publisher: Elsevier BV
Date: 02-2012
DOI: 10.1016/J.EJPB.2012.08.007
Abstract: Treatment for tuberculosis (TB) using the standard oral antibiotic regimen is effective but inefficient, requiring high drug dosing and lengthy treatment times. Three concurrent first-line antibiotics recommended by the World Health Organization (WHO) guidelines are pyrazinamide, rif icin and isoniazid. Combining these antibiotics in a novel formulation for dry powder inhalation (DPI) may facilitate rapid and efficient resolution of local and systemic infection. However, spray-dried in idually, these antibiotics were found to be physically unstable. A solution of the three antibiotics, at the WHO-recommended ratio, was spray-dried. The collected powder was assessed by a series of in vitro methods to investigate aerosol performance, particle physico-chemical characteristics and dissolution profile. Particles obtained were spherical with a surface composed primarily of rif icin, as identified by TOF-SIMS. A mass median aerodynamic diameter of 3.5 ± 0.1 μm and fine particle fraction (<5 μm) of 45 ± 3% indicated excellent aerosol performance. The combination powder was differentiated by the presence of rif icin dihydrate and the delta polymorph of pyrazinamide. Quantitative analysis indicated in idual particles contained the three antibiotics at the expected proportions (400:150:75 w/w). This excipient-free triple antibiotic DPI formulation could be used as a significant enhanced treatment for TB.
Publisher: Elsevier BV
Date: 10-2017
DOI: 10.1016/J.XPHS.2017.05.020
Abstract: This study has investigated the surface coating efficiency and powder flow improvement of a model cohesive acetaminophen powder by high-shear processing with pharmaceutical lubricants through 2 common equipment, conical comil and high-shear mixer. Effects of coating materials and processing parameters on powder flow and surface coating coverage were evaluated. Both Carr's index and shear cell data indicated that processing with the lubricants using comil or high-shear mixer substantially improved the flow of the cohesive acetaminophen powder. Flow improvement was most pronounced for those processed with 1% wt/wt magnesium stearate, from "cohesive" for the V-blended s le to "easy flowing" for the optimally coated s le. Qualitative and quantitative characterizations demonstrated a greater degree of surface coverage for high-shear mixing compared with comilling nevertheless, flow properties of the s les at the corresponding optimized conditions were comparable between 2 techniques. Scanning electron microscopy images demonstrated different coating mechanisms with magnesium stearate or l-leucine (magnesium stearate forms a coating layer and leucine coating increases surface roughness). Furthermore, surface coating with hydrophobic magnesium stearate did not retard the dissolution kinetics of acetaminophen. Future studies are warranted to evaluate tableting behavior of such dry-coated pharmaceutical powders.
Publisher: Elsevier BV
Date: 03-2008
DOI: 10.1016/J.FORSCIINT.2007.05.017
Abstract: The characterisation and comparison of pencil markings on paper is an area of questioned document analysis that has previously not received much attention. Despite this, there would be value in an examiner being able to analyse two pencil markings and coming to a conclusion about whether they were from a similar or different source. Previous studies have analysed raw materials and bulk pencil cores for purposes of characterisation and differentiation, but to date, no studies have successfully analysed pencil markings non-destructively off a paper substrate. In this work, pencils from a number of manufacturers were analysed by inductively coupled plasma mass spectrometry (ICP-MS) and time-of-flight secondary ion mass spectrometry (ToF-SIMS). Analysis of data using multivariate techniques (principal component analysis), showed that ToF-SIMS can successfully be used to analyse such pencil markings to deduce whether two markings can be differentiated, in terms of inorganic elemental composition. It was possible to discriminate between pencil markings from different manufacturers, and it was also indicated that pencils from the same manufacturer, but discrete batches, can be significantly different.
Publisher: Elsevier BV
Date: 05-2016
DOI: 10.1016/J.EJPB.2016.02.010
Abstract: L-Leucine (LL) has been widely used to enhance the dispersion performance of powders for inhalation. LL can also protect powders against moisture, but this effect is much less studied. The aim of this study was to investigate whether LL could prevent moisture-induced deterioration in in vitro aerosolization performances of highly hygroscopic spray-dried powders. Disodium cromoglycate (DSCG) was chosen as a model drug and different amounts of LL (2-40% w/w) were added to the formulation, with the aim to explore the relationship between powder dispersion, moisture protection and physicochemical properties of the powders. The powder formulations were prepared by spray drying of aqueous solutions containing known concentrations of DSCG and LL. The particle sizes were measured by laser diffraction. The physicochemical properties of fine particles were characterized by X-ray powder diffraction (XRD), differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), and dynamic vapor sorption (DVS). The surface morphology and chemistry of fine particles were analyzed by scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and time-of-flight secondary ion mass spectrometry (ToF-SIMS). In vitro aerosolization performances were evaluated by a next generation impactor (NGI) after the powders were stored at 60% or 75% relative humidity (RH), and 25°C for 24h. Spray-dried (SD) DSCG powders were amorphous and absorbed 30-45% (w/w) water at 70-80% RH, resulting in deterioration in the aerosolization performance of the powders. LL did not decrease the water uptake of DSCG powders, but it could significantly reduce the effect of moisture on aerosolization performances. This is due to enrichment of crystalline LL on the surface of the composite particles. The effect was directly related to the percentage of LL coverage on the surface of particles. Formulations having 61-73% (molar percent) of LL on the particle surface (which correspond to 10-20% (w/w) of LL in the bulk powders) could minimize moisture-induced deterioration in the aerosol performance. In conclusion, particle surface coverage of LL can offer short-term protection against moisture on dispersion of hygroscopic powders.
Publisher: Elsevier BV
Date: 08-2011
DOI: 10.1002/JPS.22547
Publisher: Springer Science and Business Media LLC
Date: 16-05-2016
DOI: 10.1038/SREP26008
Abstract: Alkaline polyphosphate has been demonstrated to be able to reduce significant wear and friction of sliding interfaces under heavy loads ( GPa) and elevated temperature (800 °C and above) conditions, e.g. hot metal manufacturing. The chemical composition and fine structure of polyphosphate lubricating film is not well understood as well as the role of alkaline elements within the reaction film at hot rubbing surface. This work makes use of the coupling surface analytical techniques on the alkaline polyphosphate tribofilm, XANES, TOF-SIMS and FIB/TEM. The data show the composition in gradient distribution and trilaminar structure of tribofilm: a shorter chain phosphate overlying a long chain polyphosphate that adheres onto oxide steel base through a short chain phosphate. The chemical hardness model well explains the anti-abrasive mechanism of alkaline polyphosphate at elevated temperatures and also predicts a depolymerisation and simultaneous cross-linking of the polyphosphate glass. The role of alkaline elements in the lubrication mechanism is especially explained. This work firstly serves as a basis for a detailed study of alkaline polyphosphate tribofilm at temperature over 600 °C.
No related grants have been discovered for John Denman.