Chemical and Biomolecular Engineering - Research Publications
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ItemRemote Control in Formation of 3D Multicellular Assemblies Using Magnetic Forces(AMER CHEMICAL SOC, 2019-05)Cell constructs have been utilized as building blocks in tissue engineering to closely mimic the natural tissue and also overcome some of the limitations caused by two-dimensional cultures or using scaffolds. External forces can be used to enhance the cells' adhesion and interaction and thus provide better control over production of these structures compared to methods like cell seeding and migration. In this paper, we demonstrate an efficient method to generate uniform, three-dimensional cell constructs using magnetic forces. This method produced spheroids with higher densities and more symmetrical structures than the commonly used centrifugation method for production of cell spheroids. It was also shown that shape of the cell constructs could be changed readily by using different patterns of magnetic field. The application of magnetic fields to impart forces on the cells enhanced the fusion of these spheroids, which could be used to produce larger and more complicated structures for future tissue engineering applications.
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ItemThiol-Reactive Star Polymers Functionalized with Short Ethoxy-Containing Moieties Exhibit Enhanced Uptake in Acute Lymphoblastic Leukemia Cells(DOVE MEDICAL PRESS LTD, 2019)PURPOSE: Directing nanoparticles to cancer cells without using antibodies is of great interest. Subtle changes to the surface chemistry of nanoparticles can significantly affect their biological fate, including their propensity to associate with different cell populations. For instance, nanoparticles functionalized with thiol-reactive groups can potentially enhance association with cells that over-express cell-surface thiol groups. The potential of such an approach for enhancing drug delivery for childhood acute lymphoblastic leukemia (ALL) cells has not been investigated. Herein, we investigate the impact of thiol-reactive star polymers on the cellular association and the mechanisms of uptake of the nanoparticles. METHODS: We prepared fluorescently labeled star polymers functionalized with an mPEG brush corona and pyridyl disulfide to examine how reactivity to exofacial thiols impacts cellular association with ALL cells. We also studied how variations to the mPEG brush composition could potentially be used as a secondary method for controlling the extent of cell association. Specifically, we examined how the inclusion of shorter diethylene glycol brush moieties into the nanoparticle corona could be used to further influence cell association. RESULTS: Star polymers incorporating both thiol-reactive and diethylene glycol brush moieties exhibited the highest cellular association, followed by those functionalized solely with thiol reactive groups compared to control nanoparticles in T and B pediatric ALL patient-derived xenografts harvested from the spleens and bone marrow of immunodeficient mice. Transfection of cells with an early endosomal marker and imaging with correlative light and electron microscopy confirmed cellular uptake. Endocytosis inhibitors revealed dynamin-dependent clathrin-mediated endocytosis as the main uptake pathway for all the star polymers. CONCLUSION: Thiol-reactive star polymers having an mPEG brush corona that includes a proportion of diethylene glycol brush moieties represent a potential strategy for improved leukemia cell delivery.
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ItemThe use of carbonic anhydrase to accelerate carbon dioxide capture processes(WILEY, 2015-01)The chemical absorption of CO2 into a monoethanolamine solvent is currently the most widely accepted commercial approach to carbon dioxide capture. However, the subsequent desorption of CO2 from the solvents is extremely energy intensive. Alternative solvents are more energy efficient, but their slow reaction kinetics in the CO2 absorption step limits application. The use of a carbonic anhydrase (CA) enzyme as a reaction promoter can potentially overcome this obstacle. Native, engineered and artificial CA enzymes have been investigated for this application. Immobilization of the enzyme within the gas absorber or in a membrane format can increase enzyme stability and avoid thermal denaturation in the stripper. However, immobilization is only effective if the mass transfer of carbon dioxide through the liquid phase to reach the immobilization substrate does not become rate controlling. Further research should also consider the process economics of large-scale enzyme production and the long-term performance of the enzyme under real flue gas conditions.
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ItemConvective transport of boron through a brackish water reverse osmosis membrane(Elsevier, 2013-10-15)In this work, cross-flow filtration experiments using a brackish water reverse osmosis polyamide membrane have been performed to gather boron rejection data as function of feed concentration, pressure, pH and salinity. Increasing transmembrane pressure increases the permeation of boron indicating that convective flow is important. This result is in contrast to the normal assumption that solution diffusion dominates in such systems. The extended Nernst-Planck equation with a Donnan-steric partition coefficient is used to analyse the transport mechanisms of both neutral boric acid and negatively charged borate ions through the RO membrane. The contribution of surface charge is experimentally determined by streaming potential measurements and the electrokinetic surface charge density is then calculated as a function of ionic strength and pH. It is found that a 0.380 nm pore radius and an effective membrane porosity of 0.05 shows good agreement with experimental data. Charge screening becomes more dominant with increasing ionic strength and this contribution is readily incorporated into the model. The study extends our understanding of the transport mechanism of boric acid and borate ions which can assist in predicting the performance of polyamide reverse osmosis membranes. It also raises questions as to the true mechanism of transport through such a membrane.
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ItemFormation of a thick aromatic polyamide membrane by interfacial polymerisation(Elsevier, 2013-02-05)Thin film composite membranes (TFCs) consist of a thin film of polymer that is responsible for high salt rejection. This layer is made via interfacial polymerisation of two monomers 1,3 phenylene diamine and trimesoyl chloride, with the membrane reported to reach a self limiting thickness of less than 200 nm. This paper reports for the first time the formation of thick free-standing aromatic polyamide membranes of greater than 50 μm in thickness via the well-known interfacial polymerisation technique. The membrane thickness as a function of polymerisation time and monomer concentration was investigated. The polyamide layer formed through interfacial polymerisation is not necessarily homogeneous, but can indeed feature areas of porosity. A mechanism for such a porous structure is proposed and discussed. The ability to form thick free-standing polyamide membranes allows bulk polymer properties to be evaluated for the first time. In particular, in this work we are able to measure the zeta potential of the membrane surface that usually faces the membrane support. We show that this surface is still negatively charged for all pH values above 4.0.
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ItemWater vapor sorption and free volume in the aromatic polyamide layer of reverse osmosis membranes(Elsevier, 2013-01-01)Thin film composite membranes consist of an ultra thin active layer of polymer that governs the membrane's salt rejection and water permeation properties. However, the fragility of the ultrathin layer makes it challenging to select a technique capable of differentiating between the properties of this layer from the supporting layer. In this study, we isolated enough active layer material to characterise the water vapour sorption and free volume cavity size as functions of water activity. The sorption data were modelled using the Guggenheim–Anderson–De Boer (G.A.B.) isotherm and from this the number of sorption sites for water was calculated to be 189×1019 per gram for the active layer from a commercial Dow Filmtec SW30 membrane and 188×1019 per gram for an aromatic polyamide material prepared in house. The activation energy for diffusion of water through the active layer of SW30 was also evaluated and found to be 6.95 kcal/mol, lower than the heat of liquefaction of water. This suggests that water does not permeate as individual molecules in the vapour state, but rather as clusters of water molecules. The free volume cavity size in the active layer as a function of moisture uptake was also investigated and the results were explained using a pore filling and pore swelling mechanism. This study sheds light on the mechanisms of water entry into the active layer, water transport through the active layer, and the corresponding response of the polymer chains, thereby giving critical insight for the development of more novel systems.
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ItemSelf-template construction of nanoporous carbon nanorods from a metal-organic framework for supercapacitor electrodes(ROYAL SOC CHEMISTRY, 2018)The morphologies and structures of nanostructured carbons generally influence their catalysis, electrochemical performance and adsorption properties. Metal-organic framework (MOF) nanocrystals usually have various morphologies, and can be considered as a template to construct nanostructured carbons with shaped nanocubes, nanorods, and hollow particles by thermal transformation. However, thermal carbonization of MOFs usually leads to collapse of MOF structures. Here, we report shape-preserved carbons (termed as CNRods) by thermal transformation of nickel catecholate framework (Ni-CAT) nanorods. Supercapacitors of CNRods treated at 800 °C were demonstrated to have enhanced performance due to their structural features that facilitate electron conduction and ion transport as well as abundant O content benefiting the wettability of the carbon materials. This may provide a potential way to explore novel carbon materials for supercapacitors with controllable morphologies and high capacitive performance.
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ItemA modelling approach to assess the long-term stability of a novel microbial/electrochemical system for the treatment of acid mine drainage.(Royal Society of Chemistry (RSC), 2018-05-17)Microbial electrochemical processes have potential to remediate acid mine drainage (AMD) wastewaters which are highly acidic and rich in sulfate and heavy metals, without the need for extensive chemical dosing. In this manuscript, a novel hybrid microbial/electrochemical remediation process which uses a 3-reactor system - a precipitation vessel, an electrochemical reactor and a microbial electrochemical reactor with a sulfate-reducing biocathode - was modelled. To evaluate the long-term operability of this system, a dynamic model for the fluxes of 140 different ionic species was developed and calibrated using laboratory-scale experimental data. The model identified that when the reactors are operating in the desired state, the coulombic efficiency of sulfate removal from AMD is high (91%). Modelling also identified that a periodic electrolyte purge is required to prevent the build-up of Cl- ions in the microbial electrochemical reactor. The model furthermore studied the fate of sulfate and carbon in the system. For sulfate, it was found that only 29% can be converted into elemental sulfur, with the rest complexating with metals in the precipitation vessel. Finally, the model shows that the flux of inorganic carbon under the current operational strategy is insufficient to maintain the autotrophic sulfate-reducing biomass. The modelling approach demonstrates that a change in system operational strategies plus close monitoring of overlooked ionic species (such as Cl- and HCO3 -) are key towards the scaling-up of this technology.
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ItemFlexible C-Mo2C fiber film with self-fused junctions as a long cyclability anode material for sodium-ion battery(ROYAL SOC CHEMISTRY, 2018)Electrospun carbon fiber films have high contact resistance at the fiber junctions, which causes poor cycling stability and limits their further improvement in energy storage performances. To eliminate the contact resistance of the film, we provide a new strategy to fuse the fiber junctions by introducing MoO2 in the fibers, which replaces the C-C interface by a more active C-MoO2-C interface at the fiber junction to promote mass transfer. MoO2 reacts with C matrix to generate Mo2C and form self-fused junctions during the carbonization process. Due to much lower charge transfer and sodium diffusion resistance, the C-Mo2C fiber film with self-fused junctions shows much better cyclability with capacity retention of 90% after 2000 cycles at a constant current density of 1 A g-1. Moreover, the Mo2C particles provide many electrochemically active sites, leading to additional improvement in sodium storage. The C-Mo2C fiber film has a capacity of 134 mA h g-1 at 1 A g-1 and a high capacity of 99 mA h g-1 even at 5 A g-1.
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ItemPolysulfides made from re-purposed waste are sustainable materials for removing iron from water(ROYAL SOC CHEMISTRY, 2018)Water contaminated with Fe3+ is undesirable because it can result in discoloured plumbing fixtures, clogging, and a poor taste and aesthetic profile for drinking water. At high levels, Fe3+ can also promote the growth of unwanted bacteria, so environmental agencies and water authorities typically regulate the amount of Fe3+ in municipal water and wastewater. Here, polysulfide sorbents-prepared from elemental sulfur and unsaturated cooking oils-are used to remove Fe3+ contaminants from water. The sorbent is low-cost and sustainable, as it can be prepared entirely from waste. The preparation of this material using microwave heating and its application in iron capture are two important advances in the growing field of sulfur polymers.