Chemical and Biomolecular Engineering - Research Publications
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ItemCrosslinked PVA based polymer coatings with shear-thinning behaviour and ultralow hydrogen permeability to prevent hydrogen embrittlement(Elsevier, 2024-02-07)An economic transition from natural gas to a hydrogen economy will require redeployment of steel pipelines and other infrastructure. Mechanisms are urgently needed to prevent embrittlement of the steel in hydrogen service. In this work, we show that poly vinyl alcohol (PVA) and poly (ethylene glycol) diglycidyl ether (PEGDGE) crosslinked polymer materials can be used as internal coatings to dramatically reduce hydrogen permeation to the steel surface. Unlike other crosslinked PVA systems, these materials are shear-thinning and thixotropic, which is an essential requirement for facile, in situ application onto existing infrastructure. A hydrogen permeability of 0.01 Barrer is achieved, which is up to 100 times lower than commercially available coating materials. Experiments show that increasing concentrations of the alkali catalyst (KOH) do not impact the permeability of the crosslinked films but can benefit the rheology by shortening the reaction time. Higher reaction ratios of PVA to PEGDGE give lower hydrogen permeability due to a higher degree of polymer crystallinity, but less favorable rheology due to slower reaction kinetics. PVA with higher molecular weight gives lower hydrogen permeability and promotes shear-thinning behaviour, while PEGDGE with higher molecular weight increased the film permeability but enhances the shear-thinning behavior with shorter reaction times.
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ItemInternal polymeric coating materials for preventing pipeline hydrogen embrittlement and a theoretical model of hydrogen diffusion through coated steel(PERGAMON-ELSEVIER SCIENCE LTD, 2022-08-26)This work develops a theoretical analysis of the coating permeability necessary for use as internal coatings of transmission pipelines to prevent hydrogen embrittlement. Internal coating materials suitable to be applied in situ on existing steel pipelines are also evaluated. Twelve different commercially available coatings; crosslinked poly (vinyl alcohol) (PVA), poly (vinyl chloride) and bisphenol A diglycidyl ether (DGEBA)/polyetheramine (D-400) epoxy coatings prepared in-house were tested. Films fabricated from two commercial epoxies had hydrogen permeability of 0.40 Barrer and 0.35 Barrer respectively, which show potential as coating materials. A hydrogen permeability of 0.0084 Barrer was achieved with a crosslinked poly (vinyl alcohol) coating, indicating that this material shows the highest potential of all coatings tested. Unsteady-state hydrogen diffusion through coated steel was then modeled to evaluate the effect of the coating film in reducing hydrogen embrittlement. The result shows that with a 2 mm PVA coating, hydrogen permeation inside the coating will take seven years to reach equilibrium and the final hydrogen concentration on the steel surface will be 44% lower than that without a coating. Greater protection can be provided if coatings can be developed with lower hydrogen permeability.
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ItemEngineered assembly of water-dispersible nanocatalysts enables low-cost and green CO2 capture(NATURE PORTFOLIO, 2022-03-10)Catalytic solvent regeneration has attracted broad interest owing to its potential to reduce energy consumption in CO2 separation, enabling industry to achieve emission reduction targets of the Paris Climate Accord. Despite recent advances, the development of engineered acidic nanocatalysts with unique characteristics remains a challenge. Herein, we establish a strategy to tailor the physicochemical properties of metal-organic frameworks (MOFs) for the synthesis of water-dispersible core-shell nanocatalysts with ease of use. We demonstrate that functionalized nanoclusters (Fe3O4-COOH) effectively induce missing-linker deficiencies and fabricate mesoporosity during the self-assembly of MOFs. Superacid sites are created by introducing chelating sulfates on the uncoordinated metal clusters, providing high proton donation capability. The obtained nanomaterials drastically reduce the energy consumption of CO2 capture by 44.7% using only 0.1 wt.% nanocatalyst, which is a ∽10-fold improvement in efficiency compared to heterogeneous catalysts. This research represents a new avenue for the next generation of advanced nanomaterials in catalytic solvent regeneration.
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ItemGas-liquid membrane contactors for carbon dioxide separation: A review(ELSEVIER SCIENCE SA, 2021-05-01)Membrane gas–liquid contactors have been developed to reduce the capital cost and energy consumption of conventional CO absorption and stripping columns. As a hybrid technology of membrane separation and amine absorption, these units can improve the gas absorption process by generating 400–1500% greater mass transfer area per unit volume leading to smaller equipment sizes. Regeneration of CO can occur within a membrane contactor below the boiling point of the solvent, leading to lower energy consumption. Over recent years, a vast array of polymeric and ceramic materials have been considered for membrane gas–liquid contactors and an array of solvents have been used including amines, potassium carbonate, ammonia and amino acids. The major technical challenge with membrane contactors is the wetting of the membrane pores with solvent, which reduces the mass transfer coefficient. However, other factors such as the choice of solvent, the placement of the solvent on the shell or lumen side and the operational temperature are also critical to success. This review describes the recent progress in membrane gas–liquid contactor technology for CO separation in terms of the materials, solvents, modules and processes and provides direction on where research can best be directed in the future to enhance the feasibility of the technology's industrial application. 2 2 2
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ItemReview of Membranes for Helium Separation and Purification(MDPI, 2017-03)Membrane gas separation has potential for the recovery and purification of helium, because the majority of membranes have selectivity for helium. This review reports on the current state of the research and patent literature for membranes undertaking helium separation. This includes direct recovery from natural gas, as an ancillary stage in natural gas processing, as well as niche applications where helium recycling has potential. A review of the available polymeric and inorganic membranes for helium separation is provided. Commercial gas separation membranes in comparable gas industries are discussed in terms of their potential in helium separation. Also presented are the various membrane process designs patented for the recovery and purification of helium from various sources, as these demonstrate that it is viable to separate helium through currently available polymeric membranes. This review places a particular focus on those processes where membranes are combined in series with another separation technology, commonly pressure swing adsorption. These combined processes have the most potential for membranes to produce a high purity helium product. The review demonstrates that membrane gas separation is technically feasible for helium recovery and purification, though membranes are currently only applied in niche applications focused on reusing helium rather than separation from natural sources.
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ItemEfficient degumming of crude canola oil using ultrafiltration membranes and bio derived solvents(Elsevier BV, 2020-01-01)Vegetable oils derived from rapeseed and its genetic variant canola, are conventionally extracted from oilseeds by means of an organic solvent, typically hexane. Concerns regarding the toxicity of hexane have meant safer and more environmentally friendly solvents such as terpenes are becoming attractive. In this research, the degumming of canola oil/terpene mixtures using ultrafiltration is considered as a critical step in such an extraction process. Polysulfone (PSF) and polyethersulfone (PES) membranes were found to be ineffective in this application, as the oil appeared to cause swelling of the membrane structure. This meant that the original flux could not be restored after cleaning. Conversely, a ceramic membrane (MWCO 5 kDa) provided stable behaviour over several cycles of operation when cleaned with pure solvent at high cross velocity at 40 °C. This membrane showed high phospholipid retention (95 ± 2%), although some oil was also retained (16 ± 3%). Cymene emerged as the most attractive of the three terpenes tested, with higher permeate flux and phospholipid rejection than limonene or pinene.
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ItemMembrane gas-solvent contactor pilot plant trials for post-combustion CO2 capture(Elsevier, 2020-04-15)Membrane gas-solvent contactors are a hybrid technology of solvent absorption with membrane separation that achieves efficient and compact carbon dioxide capture. Here, we report on a successful pilot plant trial of membrane contactor technology undertaking post-combustion carbon dioxide capture from flue gas generated by an Australian black coal fired power station. The pilot plant utilised membrane contactors to undertake CO2 absorption into 30 wt% monoethanolamine (MEA) and the subsequent solvent regeneration stage to produce a pure CO2 product. The pilot plant trials identified a commercially available non-porous poly dimethylsiloxane composite hollow fiber membrane as the most suitable for both CO2 absorption and solvent regeneration. The overall mass transfer coefficient for CO2 absorption across the membrane into the solvent was comparable to laboratory results, enabling a recovery of >90% CO2 from the flue gas. Over time the mass transfer coefficient decreased because of both solvent dilution and some MEA loss, which reduced the enhancement the reaction provides to mass transfer in the solvent boundary layer. The overall mass transfer of CO2 from the solvent into the steam sweep during solvent regeneration was greater than that observed in the laboratory for the same temperature. The energy demand of the pilot plant was higher than for conventional CO2 capture technology, given the pilot nature of the process, lack of energy integration and thermal losses from uninsulated membrane modules. Accounting for these factors, the energy duty of the membrane contactor process was evaluated to be less than 4.2 MJ/kg of CO2 captured. Critically, the pilot plant demonstrated the viability of membrane contactor technology for post-combustion carbon capture on an industrial scale.
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ItemData in brief on CO2 absorption-desorption of aqueous-based amino acid solvents with phase change behaviour(Elsevier, 2019-12-01)The data presented in this paper are related to the published research article “Development of aqueous-based phase change amino acid solvents for energy-efficient CO2 capture: The role of antisolvent” [1]. The raw and analyzed data include the equilibrium and kinetics of CO2 absorption, the density and concentration of different CO2-containing species at upper and lower liquid phases, and particle size distribution of solid particles precipitated during CO2 absorption of aqueous and aqueous-based amino acid solvents. In addition, the SEM images of solid precipitates at the end of CO2 absorption are presented. The detailed values of this phase change amino acid solvent are crucial for large-scale implementation of CO2 capture systems with phase change behavior.
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ItemPolymer of Intrinsic Microporosity (PIM-1) Membranes Treated with Supercritical CO2(MDPI AG, 2019-03-18)Polymers of intrinsic microporosity (PIMs) are a promising membrane material for gas separation, because of their high free volume and micro-cavity size distribution. This is countered by PIMs-based membranes being highly susceptible to physical aging, which dramatically reduces their permselectivity over extended periods of time. Supercritical carbon dioxide is known to plasticize and partially solubilise polymers, altering the underlying membrane morphology, and hence impacting the gas separation properties. This investigation reports on the change in PIM-1 membranes after being exposed to supercritical CO2 for two- and eight-hour intervals, followed by two depressurization protocols, a rapid depressurization and a slow depressurization. The exposure times enables the impact contact time with supercritical CO2 has on the membrane morphology to be investigated, as well as the subsequent depressurization event. The density of the post supercritical CO2 exposed membranes, irrespective of exposure time and depressurization, were greater than the untreated membrane. This indicated that supercritical CO2 had solubilised the polymer chain, enabling PIM-1 to rearrange and contract the free volume micro-cavities present. As a consequence, the permeabilities of He, CH4, O2 and CO2 were all reduced for the supercritical CO2-treated membranes compared to the original membrane, while N2 permeability remained unchanged. Importantly, the physical aging properties of the supercritical CO2-treated membranes altered, with only minor reductions in N2, CH4 and O2 permeabilities observed over extended periods of time. In contrast, He and CO2 permeabilities experienced similar physical aging in the supercritical treated membranes to that of the original membrane. This was interpreted as the supercritical CO2 treatment enabling micro-cavity contraction to favour the smaller CO2 molecule, due to size exclusion of the larger N2, CH4 and O2 molecules. Therefore, physical aging of the treated membranes only had minor impact on N2, CH4 and O2 permeability; while the smaller He and CO2 gases experience greater permeability loss. This result implies that supercritical CO2 exposure has potential to limit physical aging performance loss in PIM-1 based membranes for O2/N2 separation
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ItemOrganic solvent nanofiltration of binary vegetable oil/terpene mixtures: Experiments and modelling(ELSEVIER, 2019-03-01)Bio-derived solvents such as ρ-cymene, d-limonene and α-pinene represent feasible alternatives to n-11 hexane for the extraction of vegetable oils. However, the large-scale utilization of these solvents is 12 still limited mainly owing to their high boiling points and latent heats of vaporization. In this work, the 13 performance of composite polydimethylsiloxane/polyacrylonitrile (PDMS/PAN) organic solvent 14 nanofiltration membranes in the recovery of these solvents from their binary mixtures with canola oil 15 is investigated. The sorption isotherms of the mixtures were first studied using free-standing PDMS 16 films and the multicomponent Flory-Huggins model used to determine the resulting interaction 17 parameters. The partial solvent uptake decreased with increasing oil concentration in the mixture. On 18 the other hand, the partial oil uptake in the solvent mixture was higher than that of the pure oil which 19 was attributed to the swelling effects induced by solvents. The effects of feed concentration (10-30 20 wt. % oil), feed temperature (25-40 °C), transmembrane pressure (5-30 bar), and cross-flow velocity 21 (18-52 cm s-1) on the membrane performance were then studied in a cross-flow membrane setup. 22 Maxwell-Stefan formulations were combined with the ternary Flory-Huggins solubility model to 23 successfully describe these flux data.