Chemical Engineering Commons^™

Solvent Effect Modeling In Heterogenous Catalysis, Mehdi Zare

Theses and Dissertations

In recent years, the biorefining industry and biofuels have emerged as a major American energy sector. Biofuels are fuels produced from plant and animal material, also referred to as biomass. This includes wood products, manure, and corn, among other materials. Compared to fossil fuels, biofuels are significantly more environmentally friendly and thus pose less of a threat to environmental health. In 2019, the United States consumed around 14.54 billion gallons of ethanol and around 1.81 billion gallons of biodiesel. By 2030, the United States is expected to consume around 95 Mtoe of biofuels. In order to meet current demand and …

Degradation Of Antibiotics In Aqueous Phase Using Pms Catalytic Decomposition With Zero-Valent Iron Nanoparticles Immobilized In Sba-15, Ahdee Bluma Zeidman

UNLV Theses, Dissertations, Professional Papers, and Capstones

Zero-valent iron nanoparticles (nZVI) have been studied as an option for soil remediation and water treatment for many years. The capability of nZVI to produce oxidation/reduction processes, depending on the reaction conditions, has attracted great interest with their major drawback being reactivity loss through agglomeration. The loss in nZVI surface area has been reported to be prevented through immobilization onto a porous media (e.g., SBA-15, MCM-41, or zeolites). In this work, a mesoporous silica structure (SBA-15) is used as an nZVI supporting material to enhance its reactivity and promote peroxymonosulfate (PMS) catalytic decomposition for the degradation of antibiotics in aqueous …

Conversion Of Lignocellulose Biomass From Date Palm Waste To High Value Chemicals, Emmanuel Galiwango

Dissertations

Lignocellulose biomass has gained growing popularity because of its low cost of production compared to food crops, it solves problems of food and energy security, can grow in various climates and land, and it is CO₂ neutral. Date palm trees produce large amounts of fibrous wastes that are good sources of lignocellulose. There are over 40 million date palm trees in UAE and most of their lignocellulosic wastes (i.e., leaves, surface fibers, bunches, etc.) are currently used for low value applications such as compost or electric generation. However, the lignocellulosic components of this waste stream have the potential to …

Alternative View Of Oxygen Reduction On Porous Carbon Electrocatalysts: The Substance Of Complex Oxygen-Surface Interactions, Giacomo De Falco, Marc Florent, Jacek Jagiello, Yongqiang Cheng, Luke L. Daemen, Anibal J. Ramirez-Cuesta, Teresa J. Bandosz

Publications and Research

Electrochemical oxygen reduction reaction (ORR) is an important energy-related process requiring alternative catalysts to expensive platinum-based ones. Although recently some advancements in carbon catalysts have been reported, there is still a lack of understanding which surface features might enhance their efficiency for ORR. Through a detailed study of oxygen adsorption on carbon molecular sieves and using inelastic neutron scattering, we demonstrated here that the extent of oxygen adsorption/interactions with surface is an important parameter affecting ORR. It was found that both the strength of O2 physical adsorption in small pores and its specific interactions with surface ether functionalities in the …

Continuous Preparation And Application Of Novel Heterogeneous Catalysis, Michael B. Burkholder

Theses and Dissertations

Transition metal heterogeneous catalysts are widely used across many chemical industries to reduce waste and emissions and reduce production time while increasing rate. The prevalence of these materials results from the complex relationship between metal nanoparticles and supports affecting final catalytic performance. Rational catalyst synthesis describes the ability to precisely engineer structures through controlled preparation. Novel materials and continuous processing represent a promising approach for rational catalyst synthesis.

The application of these catalysts in continuous, multiphase processes, such as cross-coupling reactions, oxidation chemistry, and nitroreduction processes, are paramount to developing new commercial routes for high-value products. Pd/G catalysts synthesized by …

Cyclic Sequential Adsorption Desorption/Thermal-Catalytic Oxidation Of Volatile Organic Compounds: Material Development, Process Advancement/Improvement, And Numerical Modeling, Simulation And Optimization, Busuyi Ojo Adebayo

Doctoral Dissertations

"Volatile organic compounds (VOCs) are a group of useful organic chemicals but when emitted have contributed to air pollution. They affect human health, cause environmental degradation and contaminate our waters and soils, so they need to be controlled. When they exist in dilute concentrations, abatement becomes challenging, thus requiring advanced abatement methods, e.g., sequential adsorption desorption/thermal-catalytic oxidation process. The overall goal of this research was to abate dilute streams of VOCs via the process. The specific objectives were to 1) develop novel adsorbent/catalyst dual-function materials (DFMs) for the process, 2) improve the operability of a one-bed-one-column reactor configuration for the …

Microwave-Assisted Natural Gas Conversion To Value-Added Chemicals, Xinwei Bai

Graduate Theses, Dissertations, and Problem Reports (ETD)

Stranded gas is a raw gas mixture of volatile hydrocarbons where the main composition is methane. The producers flare the stranded gas at the site because the cost of collecting and transporting the gas is higher than the value of the gas itself. To reduce the waste of this natural resource, it is worthwhile to utilize the on-site stranded natural gas as feedstock to produce value-added chemicals without emitting greenhouse gas. Direct natural gas conversion process is more desirable because of lower capital investment. Methane and ethane, the two major components of natural gas, are very stable molecules that usually …

Simultaneous Activation Of Stable Molecules- Methane And Nitrogen- Using Microwave Reactor With And Without Plasma- To Produce Ethylene And Ammonia, Sarojini Tiwari

Graduate Theses, Dissertations, and Problem Reports (ETD)

The discovery of stranded natural gas around the world has made shale gas cheaper and widely accessible. This has driven the relevant research towards the direct utilization of Methane (CH4), a major component of natural gas. CH4 is a highly stable molecule, hence its activation and consequent formation of value-added chemicals in a direct and efficient manner is a relevant problem of the 21st century. All the commercial processes convert natural gas to chemicals indirectly, via the formation of syngas followed by several reactions. The conventional systems are energy intensive and one of the major contributors to green-house gas emissions. …

Understanding The Role Of Atom Trapping In The Evolution Of Hydrocarbon Transformation Catalyst Morphology, Griffin Alexander Canning

Chemistry and Chemical Biology ETDs

Converting alkanes to other, more chemically and economically valuable molecules requires catalysts that can survive elevated temperatures and highly reducing environments. These environments can cause many metal-nanoparticle based catalysts to sinter rapidly, causing a loss of activity. They must also tolerate the coke formation, as well, since coke can restrict access to active sites by gas phase molecules, thus lowering catalytic activity. While there are routes to improve both the sinter and coke resistance of catalysts, an alternative strategy is to develop a protocol for regenerating the activity of the catalyst in question when coke formation or sintering becomes problematic. …

Advanced Materials For Air Pollutants Removal In A Combustion System, Sungyoon Jung

McKelvey School of Engineering Graduate Student Theses & Dissertations

Air pollutants directly or indirectly impact human health and the environment. Large quantities of CO2, volatile organic compounds (VOCs), and particulate matter are emitted from combustion systems, and cause climate change, smog formation, and pose serious health risks. The increasing demand for the remediation of air pollutants at the source has drawn much attention to the use of advanced materials due to their high reactivities and special properties. In order to achieve the successful application of advanced materials for the remediation of problematic emissions, three aspects, (1) synthesis method, (2) characterization of materials’ structural properties, and (3) evaluation of materials’ …

Solid Materials Discovery For Thin Films, Oxide Catalysts, And Polymer Sealants, Benjamin Ruiz-Yi

Theses and Dissertations

Solid materials are made up of multiple classes, including metals, ceramics, and polymers. While each class can be developed for general purpose applications or highly specialized, discovery of new materials in order to improve upon desired properties is a non-trivial task for any type of material. A wide variety of materials encompass expansive design spaces, consisting of parameters such as chemical compositions, synthesis conditions, and post-processing. Due to this, narrowing down the design space to fit within a given figure-of-merit and economic viability becomes time consuming at best and infeasible at worst. High-throughput experimentation

High-throughput experimentation (HTE) is a methodology …

Investigation Of Oxidized Carbon Supported Au Catalysts Synthesized Via Strong Electrostatic Adsorption Of Au(En)2Cl3 For The Hydrochlorination Of Acetylene To Vinyl Chloride Monomer, Sean Reginald Noble

Theses and Dissertations

Over 20 million tons of vinyl chloride monomer (VCM) is produced every year using acetylene hydrochlorination using a supported mercuric chloride catalyst. During this process mercury is reduced and sublimes into the environment harming all living animals and humans, so carbon-supported Au catalysts have been developed in attempts to replace it. Various techniques have been used to make these catalysts including several variations of dry impregnation. In this study we investigate the ability of Strong Electrostatic Adsorption (SEA) of Au(en)₂Cl₃ onto various supports to demonstrate the ability to rationally and consistently synthesize gold catalysts with ultra-small particle …

Engineering Dopant Position In Structure-Controlled Ceo2-Zro2 Catalysts, Behnam Safavinia

LSU Master's Theses

CeO₂-ZrO₂ (CZO) nanoparticles (NPs) have application in many catalytic reactions, such as methane reformation, due to their oxygen cycling ability. Ni doping has been shown to improve the catalytic activity and acts as an active site for the decomposition of methane. In this work, Ni:CZO NPs were synthesized via a two-step co-precipitation/molten salt synthesis to compare Ni distribution, oxygen vacancy concentration, and catalytic activity relative to a reference state-of-the-art catalyst. To better understand the effects of Ni position and dispersion, and oxygen vacancy formation in these materials, the Ni concentration, reaction time, and deposition methods were varied. …

Nanostructured Metal Thin Films As Components Of Composite Membranes For Separations And Catalysis, Michael J. Detisch

Theses and Dissertations--Chemical and Materials Engineering

Novel metallic thin film composite membranes are synthesized and evaluated in this work for improved separations and catalysis capabilities. Advances in technology that allow for improved membrane performance in solvent separations are desirable for low molecular weight organic separation applications such as those in pharmaceutical industries. Additionally, the introduction of catalytic materials into membrane systems allow for optimization of complex processes in a single step. By adding a nanostructured metallic thin film to its surface, a polymer membrane may be modified to exhibit these improved properties. Using magnetron sputtering, thin metal films may be deposited on commercially available membranes to …

Catalytic Transfer Hydrogenation Reactions Of Lipids, Alexander Asiedu

Civil & Environmental Engineering Theses & Dissertations

Catalytic transfer hydrogenation (CTH) of lipids was investigated using 2-propanol as hydrogen donor for producing liquid hydrocarbons, e.g. jet fuels. The main sources of lipids selected in this study were waste cooking oil (WCO) and oil-laden algae-derived biofuel intermediate (BI). Two different catalysts were employed in this study, namely activated carbon and trimetallic-doped zeolite.

The CTH reaction was between WCO and 2-propanol in a continuous flow reactor over a packed-bed activated carbon at near atmospheric pressure. Results revealed a high level of alkenes and aromatics compounds, which are not stable and are not environmentally unfriendly. To reduce these compounds in …

A Study Of Protein And Peptide-Directed Nanoparticle Synthesis For Catalytic Materials, Abdollah Mosleh

Graduate Theses and Dissertations

Nanoparticles have received much attentions due to their unique properties that makes them suitable candidates for a broad range of applications. As the size of particles decreases, their surface area-to-volume ratio would increase which is the main cause of much attention. In addition to the size, their morphologies and compositions may also play important roles for defining unique properties. Nanoparticle synthesis include both bottom-up and top-down strategies. To control the process of inorganic nanoparticles synthesis one could follow the bottom-up approach to have atom-level control over their compositions, morphologies, phases, and sizes which is the subject of this work. Due …

Method Of Development And Use Of Catalyst-Functionalized Catalytic Particles To Increase The Mass Transfer Rate Of Solvents Used In Acid Gas Cleanup, Leland R. Widger, Cameron A. Lippert, Kunlei Liu

Center for Applied Energy Research Faculty Patents

The present invention relates to methods for improving carbon capture using entrained catalytic-particles within an amine solvent. The particles are functionalized and appended with a CO₂ hydration catalyst to enhance the kinetics of CO₂ hydration and improve overall mass transfer of CO₂ from an acid gas.

Development Of A Ws2 Catalyst For Hydrogen Evolution And Improvement Via Platinum Nanoparticle Decoration, Alexander O'Brien

Chemical Engineering Undergraduate Honors Theses

In response to a growing global need to improve utilization of green energy, the concept of renewable energy storage via electrolytic hydrogen production has gained popularity in recent years. However, the prohibitive expense of the bulk platinum catalysts currently used for the hydrogen evolution reaction prevents such a concept from being widely adoptable. This research focuses on a possible alternative catalyst, nanolayer WS₂, which is capable of promoting the hydrogen evolution reaction while maintaining economic viability. Bulk WS₂ was prepared in semiconducting, nanolayer form through liquid phase exfoliation. Prepared catalyst inks consisting of this material demonstrated successful …

Investigation Of Microwave-Assisted Synthesis Of Palladium Nanoparticles Supported On Fe3o4 As Efficient Recyclable Magnetic Catalysts For Suzuki-Miyaura Cross-Coupling, Hany A. Elazab

Chemical and Biochemical Engineering Faculty Research & Creative Works

In this research, a facile and reproducible approach was implemented for the synthesis of palladium nanoparticles supported on Fe₃O₄ with remarkable activity as an ideal catalyst for Suzuki-Miyaura cross-coupling. Magnetite supported Pd nanoparticles reveal high activity in Suzuki-Miyaura coupling reactions since they could be recycled up to seven times with the same high catalytic activity. This adopted method of catalyst synthesis has many advantages, including reproducibility and the reliability of the adopted synthetic method. The produced catalyst has unique magnetic properties to facilitate catalyst recovery from the reaction mixture by using a strong magnet as an external …

Investigation Of Microwave-Assisted Synthesis Of Palladium Nanoparticles Supported On Fe3o4 As Efficient Recyclable Magnetic Catalysts For Suzuki-Miyaura Cross-Coupling, Hany A. Elazab Dr

Chemical Engineering

In this research, a facile and reproducible approach was implemented for synthesis of palladium nano particles supported on Fe₃O₄ with remarkable activity as an ideal catalyst for Suzuki Cross – Coupling. Magnetite supported Pd nano particles reveals a high activity towards Suzuki coupling reactions as it could be recycled up to seven times with the same high catalytic activity. This adopted method of catalyst synthesis has so many advantages as reproduciblity, and reliability of the adopted synthetic method. The produced catalyst has unique magnetic properties to facilitate the catalyst recovery from the reaction mixture through using a …

Elucidation Of The Catalytic Partial Oxidation Of Methane Utilizing The One-Of-A-Kind Catalytic Shock Tube Technique, Robyn E. Smith

Dissertations and Theses

The mechanism for the catalytic partial oxidation of methane has been debated in scientific literature for over 20 years. This is a seemingly simple reaction producing CO, CO₂, H₂ and H₂O through either partial oxidation followed by complete oxidation or complete oxidation followed by reforming steps. What is happening when the reaction is allowed to occur in an environment absent of transport limitations, absent of temperature gradients and temperature changes, absent of boundary layers must be understood and, until now, has yet to be achieved in one experimental technique.

A novel method using a one …

First-Principles Study On The Catalytic Role Of Cerium Dioxide In The Conversion Of Organic Compounds, Chuanlin Zhao

LSU Doctoral Dissertations

Ceria is an earth-abundant material that has been widely used in heterogeneous catalysis, environmental catalysis, and energy applications thanks for its ability to readily convert between different oxidation states. The objective of this study is to theoretically elucidate the reaction mechanisms for the conversion of model organic compounds on ceria, in order to gain insights for the design of cost-effective and selective ceria-based catalysts. Acetaldehyde, acetic acid, and para-nitrophenyl phosphate monoester were selected as the model compounds to probe ceria surfaces. Density functional theory calculations can provide accurate predictions of adsorption and reaction energetics, which can be used to …

Investigation Of The Effects Of Solid-State Treatments On The Structure And Mobility Of Copper In Zeolites, Jiayang Wu, Laura Wilcox, Rajamani Gounder

The Summer Undergraduate Research Fellowship (SURF) Symposium

Zeolites are microporous, aluminosilicate catalysts that play an important role in industrial applications as well as studies for the fundamental understanding of catalysts for emerging reactions of interest. The introduction of aluminum into the zeolite lattice introduces a negative charge on the framework that can be balanced with extra-framework cations. The control of the aluminum distribution and the choice of charge balancing cations allows for the ability to tailor the active sites to facilitate a desired reaction. This research focuses on studying copper active sites in zeolites. Copper oxide was used as a copper precursor to introduce copper ions in …

Electronic Effect Of Platinum Alloy Catalysts On Olefin Hydrogenation Kinetics, Colin Reedy, Jeff Miller, Stephen Purdy

The Summer Undergraduate Research Fellowship (SURF) Symposium

Dehydrogenation of alkanes is the first step in transforming light hydrocarbons into liquid fuels and chemicals. This process has traditionally used platinum alloys as catalysts. Alloys are used industrially because they have a greater selectivity than monometallic platinum. Alloying platinum with an inactive promoter modifies the crystalline structure of the surface (geometric effect), and the 5d electrons in platinum responsible for chemistry (electronic effect); both have been suggested to be primarily responsible for dehydrogenation selectivity in platinum alloys. Alloy catalysts have been synthesized using early 3d transition metal promoters with the same Pt₃M crystal structure. X-Ray Absorption Spectroscopy …

Microwave-Assisted Synthesis Of Palladium Nanoparticles Supported On Copper Oxide In Aqueous Medium As An Efficient Catalyst For Suzuki Cross-Coupling Reaction, Hany A. Elazab, M. A. Sadek, Tamer T. El-Idreesy

Chemical and Biochemical Engineering Faculty Research & Creative Works

We report here a reliable green method for the synthesis of palladium nanoparticles supported on copper oxide as a highly active and efficient catalyst for Suzuki cross-coupling reaction. The experimental synthetic approach is based on microwave-assisted chemical reduction of an aqueous mixture of palladium and copper salt simultaneously using hydrazine hydrate as reducing agent. The catalyst was fully characterized using various techniques showing well-dispersed palladium nanoparticles. The catalytic activity and recyclability of the prepared catalyst were experimentally explored in the ligand-free Suzuki cross-coupling reaction with a diverse series of functionalized substrates. The synthesized Pd/CuO catalyst shows many advantages beside its …

The Catalytic Activity Of Copper Oxide Nanoparticles Towards Carbon Monoxide Oxidation Catalysis: Microwave – Assisted Synthesis Approach, Hany A. Elazab

Chemical and Biochemical Engineering Faculty Research & Creative Works

In this research, we report a simple, versatile, and reproducible method for the synthesis of copper oxide nanoparticles via microwave assisted synthesis approach. The important advantage of this catalyst is due to its important role not only in the low temperature oxidation of CO but also in potential applications in pharmaceutical and fine chemical synthesis. The results reveal that the copper oxide catalyst has particularly a remarkable high activity for CO oxidation catalysis as it was found that copper oxide (CuO) catalyst has 100% conversion of carbon monoxide into carbon dioxide at 175 oC. This also could be attributed to …

Spectro-Electrochemical Platforms For Dynamic Analyses Of Catalytic Cascade Systems, Nalin I. Andersen

Nanoscience and Microsystems ETDs

The development of spectro-electrochemical platforms that facilitate the dynamic analyses of complex catalytic cascade systems was explored in this research. These systems facilitated multiple modalities of catalysts and were used as platforms for monitoring catalytic transformations quasi-in situ. The analytical platforms allowed for the characterization of intermediates and products using surface-enhanced Raman spectroscopy (SERS). The design and fabrication of these devices proved to be reproducible, made of materials that can be manipulated for multiple applications, and incorporate fluid mechanics, electrochemistry, and multimodal catalysis. Microfluidic technology offers capabilities for understanding catalytic cascade systems by providing precise dynamic control of …

Microwave-Assisted Synthesis Of Palladium Nanoparticles Supported On Copper Oxide In Aqueous Medium As An Efficient Catalyst For Suzuki Cross-Coupling Reaction, Hany A. Elazab, M. A. Sadek, Tamer T. El-Idreesy

Chemical Engineering

We report here a reliable green method for the synthesis of palladium nanoparticles supported on copper oxide as a highly active and efficient catalyst for Suzuki cross-coupling reaction. The experimental synthetic approach is based on microwave-assisted chemical reduction of an aqueous mixture of palladium and copper salt simultaneously using hydrazine hydrate as reducing agent. The catalyst was fully characterized using various techniques showing well-dispersed palladium nanoparticles. The catalytic activity and recyclability of the prepared catalyst were experimentally explored in the ligand-free Suzuki cross-coupling reaction with a diverse series of functionalized substrates. The synthesized Pd/CuO catalyst shows many advantages beside its …

Assembling Of Niox/Mwcnts-Gc Anodic Nanocatalyst For Water Electrolysis Applications, Islam M. Al-Akraa Dr., Yaser M. Asal Mr, Saher D. Khamis Eng

Chemical Engineering

Glassy carbon (GC) electrode is intended to be modified with nickel oxide (NiOx) and multiwalled carbon nanotubes (MWCNTs) in the anodic reaction of water electrolysis. NiOx deposition time is optimized and a 5 min was enough to attain the maximum activity. A further modification of the catalyst with MWCNTs could greatly enhance its stability during continuous electrolysis. As an outcome, an energy amount of 21.7 kWh/KgO2 is minimized. Several electrochemical and materials characterization setups will be utilized to test the catalyst activity and to know its geometry and structure.

Engineering Zeolite Catalysts Through Porosity And Surface Acidity Control For Selective Production Of Light Olefins, Xin Li

Doctoral Dissertations

"Zeolites are broadly used as heterogeneous catalysts in various chemical and petrochemical industries to produce value-added chemicals and fuels, mainly due to their large surface area, acid-base properties, high thermal stability, and excellent shape-selectivity. In this dissertation, various zeolite catalysts were engineered through fine-tuning micro-meso-macro-porosity and surface acidity. The engineered zeolites were used as heterogeneous catalysts for production of light olefins such as ethylene and propylene through alcohol dehydration and hydrocarbon cracking reactions.

To control the zeolite porosity and acidity, SAPO-34@ZSM-5 and SAPO-34@Silicalite-1 composites with core-shell structure were synthesized and evaluated in ethanol dehydration reaction. Analysis of catalytic performance revealed …