Chemical and Biomolecular Engineering Research Works
Permanent URI for this collectionhttp://hdl.handle.net/1903/1656
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Item COMSOL models for working-electrode/solid-electrolyte under mechanical loadings(2025) Jung, Taeho; Song, Yueming; Valentino, Gianna M; Albertus, PaulThe attached COMSOL models simulate the mechanical state of a working-electrode/solid-electrolyte system under the following loading conditions. * Scenario I - working electrode under out-of-plane uniaxial compression * Scenario II - solid electrolyte under in-plane uniaxial compression * Scenario III - solid electrolyte under pure shearItem COMSOL fracture model(2024-08-06) Jung, Taeho; Carmona, Eric A; Song, Yueming; Albertus, PaulSolid-electrolyte (SE) fracture initiation model at the lithium/SE interface during lithium plating.Item Gradient Structural and Compositional Design of Conductive MXene Aerogels for Stable Zn Metal Anodes(Wiley, 2023-11-12) Li, Yang; Pang, Zhenqian; Ghani, Awais; Little, Joshua M.; Wang, Liping; Yang, Haochen; Zhao, Yusheng; Chen, Po-YenAqueous rechargeable zinc-ion batteries (ZIBs) are a safe and low-cost energy storage technology. However, practical ZIB exploitation faces critical challenges in achieving stable Zn metal anodes, which suffer from hydrogen evolution reaction (HER) corrosion and Zn dendrite growth. To address these challenges, a Zn2+-induced assembly process to fabricate Ti3C2Tx MXene-reduced graphene oxide aerogels with ZnO crust layers on Zn plates (abbreviated as ZnO/MG aerogel–Zn) that serve as stable Zn metal anodes is reported. By applying a constant voltage to a Zn plate, Zn2+ is gradually released to ionically crosslink MG nanosheets. After spontaneous hydrolysis and freeze-drying, a crust layer composed of ZnO nanoparticles is in situ formed. Additionally, the gradient Zn−O/Zn−F profiles across the ZnO/MG aerogel can facilitate Zn2+ transport and collectively suppress HER, enabling fast electrochemical kinetics and dendrite-free Zn deposition. Symmetric cells with ZnO/MG aerogel–Zn electrodes present stable cycling for 1200 h at 10 mA cm−2, and full cells achieve long lifespans at high rates (>500 cycles at 1.0 A g−1). Combining the advantages of an insulating protective layer and a conductive structured host, the ZnO/MG aerogel–Zn electrode with gradient structures and compositions creates synergistic advances in stable Zn metal anodes.Item Dynamic Modeling for the Design and Cyclic Operation of an Atomic Layer Deposition (ALD) Reactor(MDPI, 2013-08-19) Travis, Curtisha D.; Adomaitis, Raymond A.A laboratory-scale atomic layer deposition (ALD) reactor system model is derived for alumina deposition using trimethylaluminum and water as precursors. Model components describing the precursor thermophysical properties, reactor-scale gas-phase dynamics and surface reaction kinetics derived from absolute reaction rate theory are integrated to simulate the complete reactor system. Limit-cycle solutions defining continuous cyclic ALD reactor operation are computed with a fixed point algorithm based on collocation discretization in time, resulting in an unambiguous definition of film growth-per-cycle (𝑔𝑝𝑐). A key finding of this study is that unintended chemical vapor deposition conditions can mask regions of operation that would otherwise correspond to ideal saturating ALD operation. The use of the simulator for assisting in process design decisions is presented.Item Shape-Changing Tubular Hydrogels(MDPI, 2018-02-22) Raghavan, Srinivasa R.; Fernandes, Neville J.; Cipriano, Bani H.We describe the creation of hollow tubular hydrogels in which different zones along the length of the tube are composed of different gels. Our method to create these gels is adapted from a technique developed previously in our lab for creating solid hybrid hydrogels. The zones of our tubular gel are covalently bonded at the interfaces; as a result, these interfaces are highly robust. Consequently, the tube can be picked up, manipulated and stretched without suffering any damage. The hollow nature of these gels allows them to respond 2–30-fold faster to external stimuli compared to a solid gel of identical composition. We study the case where one zone of the hybrid tube is responsive to pH (due to the incorporation of an ionic monomer) while the other zones are not. Initially, the entire tube has the same diameter, but when pH is changed, the diameter of the pH-responsive zone alone increases (i.e., this zone bulges outward) while the other zones maintain their original diameter. The net result is a drastic change in the shape of the gel, and this can be reversed by reverting the pH to its original value. Similar localized changes in gel shape are shown for two other stimuli: temperature and solvent composition. Our study points the way for researchers to design three-dimensional soft objects that can reversibly change their shape in response to stimuli.Item Effect of a Cationic Surfactant on Microemulsion Globules and Drug Release from Hydrogel Contact Lenses(MDPI, 2019-06-06) Torres-Luna, Cesar; Hu, Naiping; Koolivand, Abdollah; Fan, Xin; Zhu, Yuli; Domszy, Roman; Yang, Jeff; Yang, Arthur; Wang, Nam SunThe present study evaluates the in vitro release of diclofenac sodium (DFNa) from contact lenses based on poly-2-hydroxyethyl methacrylate (pHEMA) hydrogels containing an embedded microemulsion to extend release duration. The oil (ethyl butyrate)-in-water microemulsion systems are prepared with two non-ionic surfactants, Brij 97 or Tween 80, together with a long-alkyl chain cationic surfactant, cetalkonium chloride (CKC). Without CKC, Brij 97 or Tween 80-based microemulsions showed average droplet sizes of 12 nm and 18 nm, respectively. The addition of CKC decreased the average droplet sizes to 2–5 nm for both non-ionic surfactants. Such significant reduction in the average droplet size corresponds to an increase in the DFNa release duration as revealed by the in vitro experiments. Contact lens characterization showed that important properties such as optical transparency and water content of Brij 97-based contact lenses with cationic microemulsions was excellent. However, the optical transparency of the corresponding Tween 80 based contact lenses was unsatisfactory. The results indicate that cationic microemulsion-laden contact lenses can benefit from combinatory effects of microemulsions and cationic surfactant at low CKC weight percentage, e.g., with the release of 70% of the drug in 45, 10, and 7 h for B97-CKC-0.45%, CKC-0.45%, and control lenses, respectively. However, the microemulsion effect on extending DFNa release became negligible at the highest CKC weight percentage (1.8%).Item Formation of Drug-Participating Catanionic Aggregates for Extended Delivery of Non-Steroidal Anti-Inflammatory Drugs from Contact Lenses(MDPI, 2019-10-10) Torres-Luna, Cesar; Koolivand, Abdollah; Fan, Xin; Agrawal, Niti R.; Hu, Naiping; Zhu, Yuli; Domszy, Roman; Briber, Robert M.; Wang, Nam Sun; Yang, ArthurThis paper focuses on extending drug release duration from contact lenses by incorporating catanionic aggregates. The aggregates consist of a long-chain cationic surfactant, i.e., cetalkonium chloride (CKC), and an oppositely charged anti-inflammatory amphiphilic drug. We studied three non-steroidal anti-inflammatory (NSAID) drugs with different octanol–water partition coefficients; diclofenac sodium (DFNa), flurbiprofen sodium (FBNa), and naproxen sodium (NPNa). Confirmation of catanionic aggregate formation in solution was determined by steady and dynamic shear rheology measurements. We observed the increased viscosity, shear thinning, and viscoelastic behavior characteristic of wormlike micelles; the rheological data are reasonably well described using a Maxwellian fluid model with a single relaxation time. In vitro release experiments demonstrated that the extension in the drug release time is dependent on the ability of a drug to form viscoelastic catanionic aggregates. Such aggregates retard the diffusive transport of drug molecules from the contact lenses. Our study revealed that the release kinetics depends on the CKC concentration and the alkyl chain length of the cationic surfactant. We demonstrated that more hydrophobic drugs such as diclofenac sodium show a more extended release than less hydrophobic drugs such as naproxen sodium.Item Two-Dimensional Zeolite Materials: Structural and Acidity Properties(MDPI, 2020-04-12) Schulman, Emily; Wu, Wei; Liu, DongxiaZeolites are generally defined as three-dimensional (3D) crystalline microporous aluminosilicates in which silicon (Si4+) and aluminum (Al3+) are coordinated tetrahedrally with oxygen to form large negative lattices and consequent Brønsted acidity. Two-dimensional (2D) zeolite nanosheets with single-unit-cell or near single-unit-cell thickness (~2–3 nm) represent an emerging type of zeolite material. The extremely thin slices of crystals in 2D zeolites produce high external surface areas (up to 50% of total surface area compared to ~2% in micron-sized 3D zeolite) and expose most of their active sites on external surfaces, enabling beneficial effects for the adsorption and reaction performance for processing bulky molecules. This review summarizes the structural properties of 2D layered precursors and 2D zeolite derivatives, as well as the acidity properties of 2D zeolite derivative structures, especially in connection to their 3D conventional zeolite analogues’ structural and compositional properties. The timeline of the synthesis and recognition of 2D zeolites, as well as the structure and composition properties of each 2D zeolite, are discussed initially. The qualitative and quantitative measurements on the acid site type, strength, and accessibility of 2D zeolites are then presented. Future research and development directions to advance understanding of 2D zeolite materials are also discussed.Item Motion of an Elastic Capsule in a Trapezoidal Microchannel under Stokes Flow Conditions(MDPI, 2020-05-17) Koolivand, Abdollah; Dimitrakopoulos, PanagiotisEven though the research interest in the last decades has been mainly focused on the capsule dynamics in cylindrical or rectangular ducts, channels with asymmetric cross-sections may also be desirable especially for capsule migration and sorting. Therefore, in the present study we investigate computationally the motion of an elastic spherical capsule in an isosceles trapezoidal microchannel at low and moderate flow rates under the Stokes regime. The steady-state capsule location is quite close to the location where the single-phase velocity of the surrounding fluid is maximized. Owing to the asymmetry of the trapezoidal channel, the capsule’s steady-state shape is asymmetric while its membrane slowly tank-treads. In addition, our investigation reveals that tall trapezoidal channels with low base ratios produce significant off-center migration for large capsules compared to that for smaller capsules for a given channel length. Thus, we propose a microdevice for the sorting of artificial and physiological capsules based on their size, by utilizing tall trapezoidal microchannels with low base ratios. The proposed sorting microdevice can be readily produced via glass fabrication or as a microfluidic device via micromilling, while the required flow conditions do not cause membrane rupture.Item Effects of Protein Unfolding on Aggregation and Gelation in Lysozyme Solutions(MDPI, 2020-09-02) Nikfarjam, Shakiba; Jouravleva, Elena V.; Anisimov, Mikhail A.; Woehl, Taylor J.In this work, we investigate the role of folding/unfolding equilibrium in protein aggregation and formation of a gel network. Near the neutral pH and at a low buffer ionic strength, the formation of the gel network around unfolding conditions prevents investigations of protein aggregation. In this study, by deploying the fact that in lysozyme solutions the time of folding/unfolding is much shorter than the characteristic time of gelation, we have prevented gelation by rapidly heating the solution up to the unfolding temperature (~80 °C) for a short time (~30 min.) followed by fast cooling to the room temperature. Dynamic light scattering measurements show that if the gelation is prevented, nanosized irreversible aggregates (about 10–15 nm radius) form over a time scale of 10 days. These small aggregates persist and aggregate further into larger aggregates over several weeks. If gelation is not prevented, the nanosized aggregates become the building blocks for the gel network and define its mesh length scale. These results support our previously published conclusion on the nature of mesoscopic aggregates commonly observed in solutions of lysozyme, namely that aggregates do not form from lysozyme monomers in their native folded state. Only with the emergence of a small fraction of unfolded proteins molecules will the aggregates start to appear and grow.