Chemical & Biomolecular Engineering
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Formerly known as the Department of Chemical Engineering.
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Item Ultra-Small Metal Nanoparticles: Aerosol- and Laser-Assisted Nanomanufacturing, Characterization, and Applications(2019) Yang, Yong; Zachariah, Michael R.; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Ultrasmall metal nanoparticles (1-10 nm) are certain to be the building blocks of the next generation of electronic, catalytic, and energy storage devices. Despite their importance, synthesizing these extremely small nanoparticles, at least in sufficient quantities to enable their industrial utility however, is challenging due to their low stability and tendency to agglomerate. Numerous techniques developed thus far typically generate metal nanoparticles in small quantities with a main difficulty in industrial scale-up being poor thermal control. This shortcoming often leads to wide size distributions, inhomogeneous dispersion, and aggregation. Thus, there is a pressing need for developing new strategies for scalable manufacturing of ultrasmall metal nanoparticles towards industrial applications. This dissertation identifies two techniques for scalable manufacturing of ultrasmall metal nanoparticles with tunable size, constituency, microstructure, and other properties: an aerosol droplet mediated approach and an ultrafast laser shock approach. The aerosol droplet mediated approach employs the fast heating and quenching nature of aerosol droplet nanoreactors containing precursor species to produce ultrasmall metal nanoparticles uniformly dispersed in polymer or graphene matrices. The fast heating and quenching nature intrinsic to the aerosol droplets is also employed to fabricate a new type of engineering material, notably high entropy alloy nanoparticles, defined as five or more well-mixed metal elements in near equimolar ratios. As an example of application, I further employ the aerosol droplets to create antimony nanoparticles incorporated carbon nanosphere network and the resulting architecture offered one of the best potassium ion battery anode performances in terms of both capacity and cycling stability. This dissertation also introduces an ultrafast laser shock technique to decorate metal nanoparticles onto carbon nanofibers (CNFs) in-situ with kinetically tunable size and surface density. A shorter laser shock enables the formation of metal nanoclusters with higher number densities and smaller sizes while longer laser shock leads to the further growth of metal nanoclusters and the achievement of their equilibrium shape. The catalytic performance towards electrocatalytic hydrogen evolution was greatly enhanced for CNF supported metal nanoclusters with a smaller size and higher number density.Item Advancements in Label-free Biosensing Using Field-Effect Transistors and Aided by Molecular Dynamics Simulations(2019) Guros, Nicholas; Klauda, Jeffery B; Balijepalli, Arvind; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Biosensors are used to characterize or measure concentrations of physiologically or pathologically significant biomarkers that indicate the health status of a patient, for example, a biomarker associated with a specific disease or cancer. Presently, there is a need to improve the capabilities of biosensors, which includes their rate of detection, limit of detection, and usability. With respect to usability, it is advantageous to develop biosensors that can detect a biomarker that is not labeled, such as with a conventional fluorescent, magnetic, or radioactive label, prior to characterization or measurement by that biosensor. Such biosensors are known as label-free biosensors and are the primary focus of this work. Biosensors are principally evaluated by two standards: their sensitivity to detect a target biomarker at physiologically relevant concentrations and their specificity to detect only the target biomarker in the presence of other molecules. The elements of biosensing critical to improving these two standards are: biorecognition of the biomarker, immobilization of the biorecognition element on the biosensor, and transduction of biomarker biorecognition to a measurable signal. Towards the improvement of sensitivity, electrostatically sensitive field-effect transistors (FET) were fabricated in a dual-gate configuration to enable label-free biosensing measurements with both high sensitivity and signal-to-noise ratio (SNR). This high performance, quantified with several metrics, was principally achieved by performing a novel annealing process that improved the quality of the FET’s semiconducting channel. These FETs were gated with either a conventional oxide or an ionic liquid, the latter of which yielded quantum capacitance-limited devices. Both were used to measure the activity of the enzyme cyclin-dependent kinase 5 (Cdk5) indirectly through pH change, where the ionic-liquid gated FETs measured pH changes at a sensitivity of approximately 75 times higher than the conventional sensitivity limit for pH measurements. Lastly, these FETs were also used to detect the presence of the protein streptavidin through immobilization of a streptavidin-binding biomolecule, biotin, to the FET sensing surface. To study the biomolecular factors that govern the specificity of biomarker biorecognition in label-free biosensing, molecular dynamics (MD) simulations were performed on several proteins. MD simulations were first performed on the serotonin receptor and ion channel, 5-HT3A. These simulations, which were performed for an order of magnitude longer than any previous study, demonstrate the dynamic nature of serotonin (5-HT) binding with 5-HT3A. These simulations also demonstrate the importance of using complex lipid membranes to immobilize 5-HT3A for biosensing applications to adequately replicate native protein function. The importance of lipid composition was further demonstrated using MD simulations of the ion channel alpha-hemolysin (αHL). The results of these simulations clearly demonstrate the lipid-protein structure-function relationship that regulates the ionic current though a lipid membrane-spanning ion channel. Finally, to demonstrate the impact of MD simulations to inform the design of FET biosensing, a strategy to use FETs to measure the ultra-low ionic currents through the ion channel 5-HT3A is outlined. This strategy leverages critical elements of 5-HT biorecognition and ion channel immobilization extracted from MD simulations for the design of the proposed FET sensing surface interface.Item DEVELOPMENT OF BILAYER ELECTROLYTE LT-SOFCs USING ALTERNATIVE BISMUTH OXIDES(2018) PESARAN, ALIREZA; Wachsman, Eric D; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)This work is primarily focused on the fabrication and performance of anode supported cells based on gadolinium doped ceria (GDC) and alternative stabilized bismuth oxide bilayer electrolyte that can operate at low temperatures (500-650 °C).The well-known bismuth-based electrolyte (ESB) undergoes ordering phenomena at temperatures ≤600°C, causing rapid decay in conductivity, and in turn the power output. As alternatives, two bismuth oxide compositions: (a) Neodymium-gadolinium stabilized bismuth oxide (NGSB) in rhombohedral phase, and (b)heavily doped composition, (Bi0.75Y0.25)1.86Ce0.14O3±δ (YCSB), with Y and Ce as co-dopants in cubic phase were evaluated in this work. For the GDC/NGSB bilayer SOFCs, thickness of GDC and NGSB layers was varied between 23-70 μm and 0-25 μm, respectively. The results showed the addition of NGSB layer was effective in blocking electronic conduction which increased the OCV compared to the baseline single layer GDC cell. Further, the relative and total thickness of the two layers showed a significant impact on the OCV of the cell at different temperatures with best performance obtained with cells with lower GDC thickness and higher NGSB thickness. For the GDC/YCSB bilayer electrolyte SOFCs, a cell with a ~ 20 μm GDC layer and a ~12-13 μm YCSB layer, OCV and MPD of the cell at 650 ℃ reached 0.833 V and 760 mW/cm2 respectively. OCV stability of this bilayer was measured for 50 hours at 625 and 600 ℃ (100 hours in total) and exceptional stability of OCV and ohmic ASR was observed. In comparison, the cell with 10GDC/ESB bilayer electrolyte showed a very rapid degradation of OCV at 600 ℃ (average hourly degradation rate of 0f -0.55%/h). and the ohmic ASR of the cell with GDC/ESB bilayer electrolyte at 600 ℃ increased by 5 times over the first 50 hours of operation mainly due to the conductivity decay of ESB. Following the stable performance of GDC/YCSB bilayer electrolyte SOFCs, effect of GDC/YCSB thickness ratio on the performance of the cell was studied. It was shown that MPD of the bilayer electrolyte cells is higher than pristine GDC based cells with reduced ohmic ASR values. Specifically, a high MPD of ~1 W/cm2 at 650℃ was achieved on a GDC(20μm)/ YCSB(12μm) bilayer electrolyte based SOFC, which is 62% higher than pristine GDC based SOFC (0.64 W/cm2). Such enhancement is due to the 9.3% improvement in OCV (from 0.791 to 0.865 V) and a considerable 36% reduction in ohmic ASR values (from 0.094 to 0.069 Ω.cm2). Finally, to achieve high power density at low temperatures (≤ 600 ℃), a thin GDC (7-8 μm)/ YCSB (2 μm) bilayer electrolyte was used, and non-ohmic ASR of the cell was drastically lowered via infiltration of Ni/GDC and LSM on anode and cathode, respectively. At 600 and 550 ℃, maximum power density (MPD) of the cell reached 1.73 and 1.25 W/cm2, respectively, significantly higher than all previously reported values using non-cobalt cathode materials. The effect of infiltrating LSM on LSM-YCSB cathode was studied by varying temperatures and partial pressure of oxygen. It was revealed that by infiltrating the LSM/YCSB cathode with LSM nanoparticles, non-ohmic ASR of cathode reduced remarkably by one order of magnitude. Stability of the infiltrated symmetrical cell at 550 ℃ was measured over a period of 500 hours with no sign of decay.Item CRYSTAL WET MILLING IN ROTOR-STATOR MIXERS(2018) Ghaderzadeh, Kanan; Calabrese, Richard V; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Wet milling in rotor-stator mixers to reduce crystal size is an emerging practice with significant potential in crystallization and milling of active pharmaceutical ingredients. The complexities of crystal breakage behavior, the turbulent nature of flow, and multiscale geometry in rotor-stator mixers have limited the understanding of the milling process in these devices. The purpose of this work is to investigate the effect of milling conditions, crystal physical properties, and mixer geometry on the milling behavior of crystals, and to introduce a mechanistic framework on which to base mill design, scale up, and operating strategies. A Silverson L4R rotor-stator mixer with a square-hole stator head was used to conduct systematic wet milling experiments. Three mill head geometries were studied. There are inline units with a standard shear gap (clearance between rotor and stator) and an enlarged shear gap, and a batch unit with a standard shear gap. Three different crystals with different elastic modulus, hardness, and fracture toughness were milled in an anti-solvent. Rotor speed and volumetric throughput were adjusted independently to vary energy input and mill head residence time. The milling rate was found to increase with higher rotor speed and lower throughput, while the ultimate particle size (maximum particle size at the end of milling) was only dependent on rotor speed. The effects of fluid agitation, particle-particle collisions, and particle-wall collisions on crystal breakage were assessed by changing particle concentration, coating the stator surfaces, and reducing rotor diameter. It was found that the concentration of particles in the slurry has a limited effect on milling rate and negligible effect on ultimate particle size. The effect of higher power input and smaller dispersion zone volume (the volume of the shear gap and stator hole regions), through changes to the mixing head geometry, showed to be more successful in concentrating the energy input, and hence, leads to higher milling rates and smaller ultimate particle size. To quantitatively explain the experimental results, a class of mechanistic models for crystal breakage were developed that consider the influence of plastic deformation, elastic deformation, and fracture toughness on breakage resistance. These models are in agreement with classical grinding theories. Based on the particle size scale, two classes of disruptive forces were studied considering either macroscale velocity (proportional to rotor tip speed) or inertial subrange turbulent eddy velocity (given by Kolmogorov’s inertial subrange model). Four cohesive force definitions were studied, each with different dependence on physical properties and particle size. The disruptive and cohesive forces were employed to construct eight different correlations for ultimate crystal size and its rate of approach. Model discrimination is based on comparison to the wet milling experimental data. The best-fitting model was based on the combination of inertial subrange model as the disruptive force and elastic-plastic deformation model as the cohesive force. For geometrically similar devices, a dimensionless comminution number was developed (ratio of disruptive to cohesive forces) to aid physical interpretation and scale up/down efforts. For devices without geometric similarity, the concept of local energy dissipation rate, defined as the power draw of the mixer per mass of fluid in shear gap and stator slot regions (calculated through computational fluid dynamics simulations), was introduced and exploited to compare the data from different mixers with different geometries. This approach was successful in correlating the maximum stable particle size resulting from wet milling of different crystals in a Silverson L4R inline mixer with standard and enlarged shear gap, and in a Silverson L4R batch mixer at different rotor speeds. The mechanistic theory is further utilized to provide breakage kernels based on probability of collision and collision rate theories. Application of the breakage functions to predict the milling rate as well as their implementation within a population balance framework is discussed.Item REVISITING THE ELECTROCHEMICAL STABILITY WINDOW OF SOLID ELECTROLYTES FOR THE DEVELOPMENT OF BULK-TYPE ALL-SOLID-STATE LITHIUM BATTERIES(2018) Han, Fudong; Wang, Chunsheng; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Bulk-type all-solid-state lithium-ion batteries (ASSLIBs) are being considered as the ultimate solution for safe lithium-ion batteries due to the replacement of volatile and flammable liquid electrolytes by nonflammable inorganic solid electrolytes (SEs). Significant advances have been made in achieving superionic SEs with a wide electrochemical stability window (ESW) from 0 to 5 V. The ESW of solid electrolytes was usually measured from the Li/SE/inert metal semi-blocking electrode. Because of the wide ESW, solid electrolytes hold great promise for high energy density batteries with high columbic efficiency and long cycle life. In this dissertation, we challenge the claimed ESW of solid electrolytes. The conventional method to measure ESW provides an overestimated value because the kinetics of the electrochemical decomposition reaction is limited in the semi-blocking electrode. A novel experimental method using Li/SE/SE+carbon cell is proposed to approach the intrinsic stability window of solid electrolytes. The ESWs of Li10GeP2S12 (LGPS) and Li7La3Zr2O12 (LLZO), the most promising SE for sulfide and oxide electrolytes respectively, are examined using the novel experimental method. The results suggest that both SEs have much narrower electrochemical stability window than what was previously claimed. The cathodic and anodic decomposition products for both electrolytes are also characterized. The measured stability window and the decomposition products agree well with the calculated results from first principles. The reversible decompositions of LGPS at both high and low voltages enable the realization of a battery made from a single material. The electrochemical decompositions of the SEs in ASSLIBs can lead to large interfacial resistances between electrode and electrolyte. The interfacial resistances arising from the decomposition of SEs have been ignored in previous research efforts because the batteries are cycled within the “claimed” stable window of SEs. Suppressing the (electro)chemical reactions between LiCoO2 cathode and LLZO electrolyte by engineering their interphase enables a high performance all-ceramic lithium battery. By taking advantage of the electrochemical decomposition of SEs, an effective approach to suppress Li dendrite formation in sulfide electrolyte is also demonstrated.Item FUNCTIONAL PARTICLE GENERATION BY AEROSOL-ASSISTED PROCESSES(2018) Liang, Yujia; Ehrman, Sheryl H; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Aerosol-assisted processes are continuous with short residence times, simple operating procedures, and facile equipment requirements. They are scalable and promising for fabrication of functional particles as conductive pastes in solar cell metallization and interference packaging, electrode materials in energy storage devices, and photocatalysts in energy conversion. Although aerosol-assisted processes have long been used in manufacturing and their fundamentals have been intensively explored, further investigation is still required to better understand the particle formation mechanisms of different aerosol-assisted processes. In this dissertation, three different aerosol-assisted processes are investigated, spray pyrolysis, colloidal spray pyrolysis (CSP), and spray drying. These processes can be conducted under mild reaction conditions with simple operation procedures. The product particles are controllable. The effects of process variables on the product particles are studied. Furthermore, the prospects of applying these three aerosol-assisted processes in generating functional particles in applications, including solar cell metallization, battery, and photocatalysis are assessed. Part 1) includes Chapters 3-5. I first present Cu-Sn binary particle generation by spray pyrolysis. Through studying the particle oxidation behaviors under different reaction conditions, the Cu-Sn binary particles exhibit high oxidation-resistance. The one-dimensional and two-dimensional structures fabricated by direct printing inks containing Cu-Sn powders display low resistivity. They all suggest that Cu-Sn binary particles produced by spray pyrolysis are promising materials in the inks in printed electronics and in the conductive pastes in solar cell metallization and interference packaging. In Part 2), Chapters 6, a novel aerosol-assisted process, CSP, is developed. This process addresses one restriction of conventional spray pyrolysis which can only be used to fabricate particles from precursor solutions containing high-solubility salts. By applying CSP, tin@carbon (Sn@C) composite particles are produced with controllable interior structures. These composite particles exhibit high-performance as the anode materials for Li-ion and Na-ion batteries. In Part 3), Chapter 7, spray drying is utilized to fabricate photocatalysts from precursor solutions containing SnO2 colloids and edge-oxidized graphene oxide (eo-GO) sheets. The particle morphology, element distribution, and band structures were investigated by various tools. The photocatalytic activity of the composite particles is five times that of commercialized TiO2 (P25) in reducing CO2 into CH4.Item Multilayered Spheres, Tubes, and Surfaces Synthesized by "Inside-Out" Polymerization(2017) Zarket, Brady; Raghavan, Srinivasa R; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Numerous materials in nature, including eggs, onions, spinal discs, and blood vessels, have multiple layers. Each layer in these materials has a distinct composition and thereby a unique function in the overall material. Our work is motivated by the need to find a simple, versatile route for the synthesis of such multilayered materials. Toward this goal, we have devised a technique termed “inside-out polymerization” to synthesize multilayered materials with precise control over the composition and thickness of each layer. Each layer is a crosslinked polymer gel and it grows from the surface of the previous layer, with this growth being controlled by precursor molecules present in the core of the structure. Using this technique, we synthesize multilayer structures in three different geometries, as described below. First, we outline our technique and use it to create multilayered polymer capsules. In particular, we create interesting capsules with concentric layers of non-responsive and stimuli-responsive polymers. The thickness of the stimuli-responsive layer varies sharply due to the stimulus while the non-responsive layer remains at the same thickness. In addition, the permeability of small molecules through the stimuli-responsive layers is also altered. This means that these multilayered capsules could be used to conduct pulsatile release of solutes such as drugs or other chemicals. In addition, we also show that multilayered capsules exhibit improved mechanical properties compared to those of the fragile core. Next, we extend our technique to the synthesis of multilayered polymer tubes. Our technique provides precise control over the inner diameter of the tube, the number of layers in the tube wall, and the thickness and chemistry of each layer. Tubes can be patterned with different polymers either in the lateral or longitudinal directions. Patterned tubes based on stimuli-responsive polymers exhibit the ability to spontaneously change their lumen diameter in response to stimuli, or to convert from a straight to a curled shape. On the whole, these tubes mimic several features exhibited by blood vessels like veins and arteries. In our last study, we use our technique to create hair-like structures that grow outward from a base polymer gel. The diameter, length, and spacing of hairs can all be tuned. The addition of hairs serves to increase the net surface area of the base gel by nearly 10-fold. This increase is comparable to the surface area increase provided by hairs called “villi” on the inner walls of small intestines. In accordance with the increased surface area, hairy surfaces extract solutes from a solution much faster than a bare surface. We also impart stimuli-responsive properties to the hairs (e.g., magnetic properties), and we show that hairy gels can be induced to fold into tubes with hairs on the outside or inside. The latter mimics the structure of the small intestine.Item Electrically Induced Gelation, Rupture, and Adhesion of Polymeric Materials(2017) Gargava, Ankit; Raghavan, Srinivasa R; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)There has been considerable interest in developing stimuli-responsive soft materials for applications in drug delivery, biosensing, and tissue engineering. A variety of stimuli have been studied so far, including temperature, pH, light, and magnetic fields. In this dissertation, we explore the use of electric fields as a stimulus for either creating new soft materials or for rupturing existing ones. Our materials are based typically on biocompatible polymers such as the polysaccharides alginate, chitosan, and agarose. We also discuss the advantages and disadvantages of electric fields over other stimuli. First, we describe the use of electric fields to form transparent and robust alginate gels around an initial mold made of agarose. Moreover, we can melt away the agarose by heat, leaving us with hollow alginate tubes. In our technique, a tubular agarose mold with dissolved calcium chloride (CaCl2) is placed in a solution of sodium alginate. A voltage of ~ 10 V is then applied, with the mold as the anode and the container as the cathode. As the Ca2+ ions migrate from the mold towards the cathode, they contact the alginate chains at the mold surface. In turn, the Ca2+ crosslinks the alginate chains into a gel, and the gel grows outward with time. The technique can be used to grow multiple layers of alginate, each with a different content, and it is also safe for encapsulation of biological species. Complex tubular structures with multiple branches and specific patterns can be created. Next, we report that electric fields can be used to rupture particles formed by ionic complexation. The particles under study are typically in the microscale (~ 200 µm radius) and are either uniformly crosslinked microbeads (e.g., alginate/Cu2+) or microcapsules formed by complexation of oppositely charged polymers (alginate and chitosan). When these particles are placed in aqueous solution and subjected to an electric field of about 10 V/cm (applied remotely, i.e., electrodes not in contact), the particles rupture within about 5 min. A possible mechanism for the electric-field-induced disruption is discussed. We also use the above particles to create electrically actuatable valves, where the flow of a liquid occurs only when the particle blocking the flow is disrupted by the field. In our final study, we show that polyelectrolyte gels and beads can be rapidly induced to adhere by an electric field. We typically work with crosslinked acrylate hydrogels made with cationic co-monomers, and anionic beads made by contacting alginate with Ca2+. When the cationic gel (connected to an anode) is contacted for just a few seconds with the anionic bead (connected to a cathode) under a voltage of ~ 10 V, the two form a strong adhesive bond. When the polarity of the electrodes is reversed, the phenomenon is reversed, i.e., the gel and bead can be easily detached. We suggest that the adhesion is due to electrophoretic migration of polyelectrolyte chains, resulting in the formation of polyion complexes. Applications of this reversible adhesion are discussed for the pick-up and drop-off of soft cargo, and for the sorting of beads.Item REACTION NETWORK ANALYSIS FOR THIN FILM DEPOSITION PROCESSES(2016) Ramakrishnasubramanian, Krishnaprasath; Adomaitis, Raymond; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Understanding the growth of thin films produced by Atomic Layer Deposition (ALD) and Chemical Vapor Deposition (CVD) has been one of the most important challenge for surface chemists over the last two to three decades. There has been a lack of complete understanding of the surface chemistry behind these systems due to the dearth of experimental reaction kinetics data available. The data that do exist are generally derived through quantum computations. Thus, it becomes ever so important to develop a deposition model which not only predicts the bulk film chemistry but also explains its self-limiting nature and growth surface stability without the use of reaction rate data. The reaction network analysis tools developed in this thesis are based on a reaction factorization approach that aims to decouple the reaction rates by accounting for the chemical species surface balance dynamic equations. This process eliminates the redundant dynamic modes and identifies conserved modes as reaction invariants. The analysis of these invariants is carried out using a Species-Reaction (S-R) graph approach which also serves to simplify the representation of the complex reaction network. The S-R graph is self explanatory and consistent for all systems. The invariants can be easily extracted from the S-R graph by following a set of straightforward rules and this is demonstrated for the CVD of gallium nitride and the ALD of gallium arsenide. We propose that understanding invariants through these S-R graphs not only provides us with the physical significance of conserved modes but also give us a better insight into the deposition mechanism.Item ENGINEERING HIERARCHICAL MESO-/MICROPOROUS LAMELLAR ZEOLITES WITH VARIABLE TEXTURAL AND CATALYTIC PROPERTIES(2016) EMDADI, LALEH; Liu, Dongxia; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Meso-/microporous zeolites combine the charactersitics of well-defined micropores of zeolite with efficient mass transfer consequences of mesopores to increase the efficiency of the catalysts in reactions involving bulky molecules. Different methods such as demetallation and templating have been explored for the synthesis of meso-/microporous zeolites. However, they all have limitations in production of meso-/microporous zeolites with tunable textural and catalytic properties using few synthesis steps. To address this challenge, a simple one-step dual template synthesis approach has been developed in this work to engineer lamellar meso-/microporous zeolites structures with tunable textural and catalytic properties. First, one-step dual template synthesis of meso-/microporous mordenite framework inverted (MFI) zeolite structures was investigated. Tetrapropyl ammonium hydroxide (TPAOH) and diquaternary ammonium surfactant ([C22H45-N+(CH3)2-C6H12-N+(CH3)2-C6H13]Br2, C22-6-6) were used as templates to produce micropores and mesopores, respectively. The variation in concentration ratios of dual templates and hydrothermal synthesis conditions resulted in production of multi-lamellar MFI and the hybrid lamellar-bulk MFI (HLBM) zeolite structures. The relationship between the morphology, porosity, acidity, and catalytic properties of these catalysts was systematically studied. Then, the validity of the proposed synthesis approach for production of other types of zeolites composites was examined by creating a meso-/microporous bulk polymorph A (BEA)-lamellar MFI (BBLM) composite. The resulted composite samples showed higher catalytic stability compared to their single component zeolites. The studies demonstrated the high potential of the one-step dual template synthesis procedure for engineering the textural and catalytic properties of the synthesized zeolites.