Steven Mullens

Aqueous tape casting of yttria stabilised zirconia using natural product binder

Abstract A new and simple tape cast process has been developed for e.g. the fabrication of YSZ-electrolyte for solid oxide fuel cells (SOFCs). The method is environmentally friendly since it is water-based and uses a natural compound as a binder. The tape cast suspension was formulated taking into account a maximal solids loading, a minimum of organic compounds, colloidal stability, rheological and wetting properties. Green sheets of variable thickness (50–400 μm) have been prepared. After sintering, dense and defect-free electrolyte material, as required for SOFCs, was obtained. The microstructure and the surface of the sintered sheet material were characterised with FESEM.

Structured catalysts for methanol-to-olefins conversion: a review

Conversion of methanol to light olefins is a promising alternative for the conversion of new feed-stocks such as gas, coal or biomass to ethylene and propylene via the methanol-to-olefins (MTO) process. During the last decade, the use of structured catalysts in this reaction has received increasing attention. The effect of such structured catalysts on the stability and selectivity is discussed in this review. The reaction and coking mechanism show the importance of good mass transfer properties of the catalyst in the MTO reaction. Important aspects such as thickness of the coating, crystal size of the zeolite and architecture of the support on the mass transfer properties of the final catalyst are highlighted. An overview of the results of structured catalysts used in the MTO reaction is presented.

Vancomycin release from poly(d,l-lactic acid) spray-coated hydroxyapatite fibers

The influence of the poly(D,L-lactic acid) (PDLLA) coating thickness on the in vitro vancomycin release from a hydroxyapatite (HA) carrier was studied. Microporous HA fibers with a porosity of 51 v% and an average pore diameter of 1.0 μm were fabricated by a diffusion-induced phase separation technique. They were loaded with 38 mg vancomycin hydrochloride (VH)/gHA, and their cylindrical shape enabled the application of the spray coating technique for the deposition of uniform PDLLA coating thicknesses, varying from 6.5 μm to 28 μm. The resulting in vitro VH release varied from a complete release within 14 days for 6.5 μm coatings to a release of 23% after 28 days for 28 μm coatings. It was clear that the VH release rate from a HA fiber can be adjusted by varying the PDLLA coating thickness. Microbiological tests of these fibers against a methicillin-resistant Staphylococcus aureus (MRSA) isolate pointed to the importance of the initial burst release and confirmed that the released antibiotics had the potential to interfere with S. aureus biofilm formation.

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.

Implantable (Bio)Polymer Coated Titanium Scaffolds: A Review

In the current review we aim to give an overview of the state of the art of the research on (bio)polymer functionalised titanium implants for bone tissue engineering applications. After a short introduction on bone tissue engineering and the requirements the applied materials have to meet, an extensive discussion on titanium in bone tissue engineering will be given. Starting with a short description of both the titanium bulk and surface properties, the requirement for surface modified titanium will be highlighted. The discussion will encompass inorganic and organic chemical modifications and a combination thereof with a focus on the organic modifications. Within the latter type of modification, physical adsorption, physical incorporation and covalent immobilisation will be compared. In the final part of the review an overview will be given of the fabrication and characterisation of three-dimensional titanium scaffolds.

Ceramic Foams Coated with Zeolite Crystals

Ceramic foams can be used as filters, dust collectors, light weight components and catalyst carriers. They can be produced by a variety of techniques. The performance of ceramic foams will be strongly improved when their mechanical properties are improved. For this reason, we produced ceramic foams both by a modified reaction bonded (RB) replica technique and by gel casting. With both methods, reticulated foam structures with enhanced mechanical strength were obtained. Zeolites are a special type of materials that are characterized by high catalytic properties. They can be brought on a structured carrier by dip and slurry coating. Nevertheless, in situ coating has as main advantage that the support is used as the base for nucleation. This results in the formation of a chemical bond between the zeolite crystals and the support. The goal of this contribution is twofold: at first we demonstrate how Al2O3 foams with improved mechanical strength can be produced both by the modified RB-alumina replica technique and by gel casting. Secondly, it is shown that these ceramic foams can be coated with (silicalite) zeolite crystals by insitu crystallization from a precursor sol. The two-layer material combinations have been characterized with FESEM, XRD, CT (computer assisted tomography), IA (Image Analysis) and by mechanical tests.

Improving the efficiency of the Diels–Alder process by using flow chemistry and zeolite catalysis

The industrial application of the Diels–Alder reaction for the atom-efficient synthesis of (hetero)cyclic compounds constitutes an important challenge. Safety and purity concerns, related to the instability of the polymerization prone diene and/or dienophile, limit the scalability of the production capacity of Diels–Alder products in a batch mode. To tackle these problems, the use of a high-pressure continuous microreactor process was considered. In order to increase the yields and the selectivity towards the endo-isomer, commercially available zeolites were used as a heterogeneous catalyst in a microscale packed bed reactor. As a result, a high conversion (≥95%) and endo-selectivity (89 : 11) were reached for the reaction of cyclopentadiene and methyl acrylate, using a 1 : 1 stoichiometry. A throughput of 0.87 g h−1 during at least 7 h was reached, corresponding to a 3.5 times higher catalytic productivity and a 14 times higher production of Diels–Alder adducts in comparison to the heterogeneous lab-scale batch process. Catalyst deactivation was hardly observed within this time frame. Moreover, complete regeneration of the zeolite was demonstrated using a straightforward calcination procedure.

Characterization and analysis of the adsorption immobilization mechanism of β-galactosidase on metal oxide powders

Immobilization of the enzymes plays a vital role in enhancing their applicability in a wide range of applications, thus ensuring the use of sustainable enzymatic processes over the conventional chemical processes on an industrial scale. This study provides the background information for the selection and screening of inorganic metal oxide (MO) powders for their use as fillers in mixed matrix membranes for enzyme immobilization as the future aim. A total of 13 MOs, ranging in size from 0.01 μm to 3 times higher than ZrO2 (used as a reference MO in this study). Upon heat treatment at 900 °C, up to 15%, 52% and 42% decline was observed in the amount of immobilized enzyme in case of alumina metal oxides (MOs), ZrO2 and TiO2, respectively. The results suggested that both isoelectric point and surface area of the MO influence the immobilization. The most important observation in this study was that the bonding of the enzyme to the MO surface seems to be mediated by the bonding/interaction of the buffer to the enzyme.

Catalyst design with porous functional structures

The chemical industry is experiencing important changes. The driving force for these changes is a growing need to improve competitiveness and consolidate market positions while complying with the regulations for safeguarding human health, and the environment. Currently, what is known as “green chemistry” or “sustainable technology” is at the heart of the changes the chemical industry is undergoing. Catalysis and materials science will play an important role in this new approach. One domain with specific relevance is porous ceramics and metals, substrates with pores sizes ranging from vacancies at the atomic level to macro pores with sizes of millimeters. There are plenty of emerging applications for porous functional components. Each application will specify the window of properties of the porous material. A technology assessment of the developed porous materials and powder processing techniques for their use as catalyst or membrane system will be presented, limited to inorganic porous materials which can be synthesized by dry and wet powder processing methods. The applications overview for porous materials is focused on macroporous components with a designed functional coating.

In vitro dissolution behavior of custom made CaP scaffolds for bone tissue engineering

The degradation rate of custom made calcium phosphate scaffolds, designed for bone tissue engineering applications, influences the healing process of critical size bone defects. An optimal degradation rate exists at which the neo-formed bone replaces the CaP (calcium phosphate) scaffold [1]. Consequently investigating the complex degradation behavior (dissolution, reprecipitation, osteoclast activity) of custom made CaP structures gains interest. In this work different in vitro dissolution experiments were performed to study the degradation behavior of 4 by composition different calcium phosphates. Ideally these experiments should have a predictive power regarding the in vivo degradation behavior. In vitro dissolution tests still lack standardization. Therefore this study focuses on the influence of two dissolution constraints: (i) the material’s macrostructure (porous - dense), (ii) the regenerated fluid flow (bath shaking - perfusion). From 4 different CaP compositions porous structures and as a reference dense disks were produced, using the same starting powder and heat treatment. To compare the different dissolution tests, all data was normalized to the CaP surface area. Results show that besides the structural appearances of the CaP structures, also the design of the dissolution test influences the in vitro dissolution behavior. Moreover there is a need to take the morphology of the dissolved material into account. The CaP perfusion tests show dissolution dynamics that resemble the in vivo reality more closely than the shaking bath experiments.