Catalysis and Reaction Engineering Commons^™

Elucidating Structure–Reactivity Relationships In Ni-Catalyzed Co2 Methanation, Majed Alam Abir

Graduate Theses, Dissertations, and Problem Reports (ETD)

The catalytic hydrogenation of carbon dioxide (CO₂) to methane represents a promising strategy for carbon utilization and renewable energy storage within power-to-gas systems. When coupled with hydrogen derived from renewable electricity, CO₂ methanation enables the conversion of intermittent energy sources into storable and transportable chemical fuels compatible with existing natural gas infrastructure. Nickel-based catalysts have emerged as leading candidates for this reaction due to their high activity towards CO₂ methanation, abundance, and cost. However, the performance and long-term stability of Ni catalysts are strongly influenced by catalyst support properties, Ni nanoparticle size, and promoter effect, and …

Modeling And Simulation Of A Process For Upcycling Of Low-Density Polyethylene Plastic Waste To Ethylene, Xiaoyan Wang

Graduate Theses, Dissertations, and Problem Reports (ETD)

Ethylene is one of the most widely produced petrochemicals, with an estimated global output of 180 million metric tons in 2022. Approximately 82 million metric tons of ethylene are used annually for plastic production, primarily for polyethylene (PE), as well as polypropylene (PP) and polyvinyl chloride (PVC). The CO₂ emissions associated with PE production were approximately 14 million metric tons in 2022. Globally, an estimated 70 million metric tons of PE are produced and consumed each year, with the majority (~79%) ending up in landfills or the environment.

This project proposes a novel process in which waste low-density polyethylene (LDPE) …

Engineering Nanomaterials From Phase-Change Biological Materials Reacting With Carbon Dioxide, Qingyang Li

Graduate Theses, Dissertations, and Problem Reports (ETD)

The current global situation concerning CO2 emissions is increasingly alarming, with rising concentrations of CO2 significantly worsening climate change and global warming. Atmospheric CO2 levels are now at their highest in millions of years, driving a host of catastrophic effects, including but not limited to extreme weather events, rising sea levels, ocean acidification, disrupted ecosystems, deteriorating air quality, respiratory health issues, heat-related illnesses, threats to food and water security, and escalating social and geopolitical tensions. To keep global warming to no more than 1.5°C higher than that of pre-industry – as called for in the Paris Agreement – emissions need …

Microwave-Assisted Reduction Of Critical Metal Oxides From E-Waste Mixture, Kurundu Shavinka Jayasekera

Graduate Theses, Dissertations, and Problem Reports (ETD)

The efficient recovery of critical metals such as tantalum (Ta), manganese (Mn), gallium (Ga), and indium (In) from electronic waste (e-waste) is essential for resource sustainability and environmental protection. This research uses microwave-assisted treatment to investigate the carbothermal reduction of these four specific metals from their oxides in a simulated e-waste mixture, with carbon black serving as both a microwave coupling and reduction agent. Microwave processing is used specifically because it offers a rapid and energy-efficient alternative to conventional thermal methods, with the benefits of intrinsic heating and selective heating of materials. The first experiments centered on understanding the effects …

Membrane Reactor Modeling And Optimization For Hydrogen Production, Ayooluwa Tomiwa Akintola

Graduate Theses, Dissertations, and Problem Reports (ETD)

There has been an ongoing trend toward cleaner fuels for more environmentally benign forms of energy generation. Recently, hydrogen has been identified as a clean fuel for energy generation. However, the most established, efficient, and widely utilized technique for producing hydrogen remains the steam methane reforming (SMR) in the presence of catalyst. Unlike other fossil fuels, utilizing methane from natural gas in an SMR process to produce hydrogen emits less, but yet a notable sum of carbon dioxide. Furthermore, the endothermic nature of SMR reactions imply that there is a high energy requirement to obtain a substantial amount of hydrogen …

Investigation Of Space Charge Effects On Co2 Electrocatalytic Reduction On Gd-Doped Ceria Via Scanning Kelvin Probe And Model-Based Bayesian Analysis, Alejandro Mejia

Graduate Theses, Dissertations, and Problem Reports (ETD)

In studying novel energy conversion and storage systems, such as high-temperature electrolysis, numerous underlying fundamental physical processes remain unclear or inadequately understood. Among these, the modeling and comprehension of surface reaction mechanisms, coupled with the intricate effects of space‑charge interfaces, remains an unclear and challenging area of research.

The work of this dissertation involves the development of a 2D finite element analysis model, leveraging the robust MOOSE framework from INL. This model, featuring inhomogeneous defect thermodynamics for near-surface chemistry, formulated through Poisson‑Cahn variational theory, has been exploited for studying the electrocatalytic reduction of CO₂ on gadolinia doped ceria. The …

Investigation Of Synergistic Effect Between Polystyrene And Polyethylene Under Conventional Thermal Heating And Microwave Heating, Thang Luong

Graduate Theses, Dissertations, and Problem Reports (ETD)

Single-use plastics (Low Density Polyethylene, LDPE; Polystyrene, PS; Polypropylene, PP) are increasingly used in the modern world, with their usage growing every year. An effective method to manage the resulting waste is urgently needed, as landfilling and incineration have proven harmful to the environment in the long term. Mechanical recycling may not maintain the desirable characteristics of the single-use plastics through several cycles. Pyrolysis emerges as a promising approach to address plastic waste. Given that single-use plastic waste often comes in a mixture, combining plastic in the feedstock is a viable solution to effectively convert these polymers altogether to gain …

Applying Thermal And Microwave Heating For Natural Gas Conversion To Value-Added Chemicals Over Zeolite-Supported Catalysts, Ashley Marie Caiola

Graduate Theses, Dissertations, and Problem Reports (ETD)

The world’s demand for natural gas has been consistently growing over the past few decades. Natural gas is considered a potential alternative to oil and coal because of its ability to burn cleaner. Although not completely emission-free, it has dominated the energy industry by providing a continuous supply of cheap fuel. Currently, natural gas makes up 41% of North American energy production. The conversion of natural gas to value-added chemicals typically involves the indirect production of synthesis gas (syngas) as an intermediate before the production of the desired product. Steam reforming and partial oxidation are two of the most common …

Ambient Ammonia Synthesis Via Microwave-Catalytic Materials And Plasma Chemistry, Siobhan Brown

Graduate Theses, Dissertations, and Problem Reports (ETD)

Ammonia is critical to supporting human life on earth because of its use as fertilizer. The Haber-Bosch process to produce ammonia has been practiced for over 100 years. This process operates at high pressure and temperature to overcome the thermodynamic and kinetic limitations of the ammonia synthesis reaction thus researchers have tried to overcome it for decades. At present this process represents 1% of global energy usage and 2.5% of global CO₂ emissions. The proposed chemical looping ammonia synthesis approach seeks to reduce the environmental impact of this critical process and to elucidate microwave-catalytic principles.

This research aims to …

Microwave-Assisted Ammonia Synthesis Over Cs-Ru/Ceo2 Catalyst, Alazar Kesete Araia

Graduate Theses, Dissertations, and Problem Reports (ETD)

Ammonia synthesis is one of the greatest innovations of the 20^th century with extensive applications from fertilizers to intermediates for nitrogen-containing chemicals and pharmaceuticals. Annually, more than 242 million tons of ammonia is produced globally, supporting approximately 27% of the world’s population. One of the fast-growing applications for ammonia is as H₂ energy carrier due to its high energy storage capacity, considered to be a decarbonized energy source. The low volumetric energy density and incompressibility makes Hydrogen a non-preferable energy carrier; an alternative carrier becomes a requirement. Ammonia possesses unique property as an energy-dense carrier to store and …

Thermochemical Water-Splitting Using Novel High-Entropy Perovskite Oxides, Hector Alexis De Santiago Hernandez

Graduate Theses, Dissertations, and Problem Reports (ETD)

In this project, we designed, synthesized, and tested the transformative (La_0.8Sr_0.2)(Mn_[1-x]/3Fe_[1-x]/3Co_xAl_[1-x]/3)O₃ (0 ≤ x ≤ 1.0) high-entropy perovskite oxides (HEPOs) as redox active oxygen carriers for thermochemical hydrogen production with improved stability, kinetics, and H₂ yield. The developed HEPOs form an R3c (hexagonal) phase and were successfully synthesized using both the Pechini and solid-state reactions with the latter synthesis being the primary source for testing. These innovative perovskites demonstrated an improved kinetics with oxygen surface exchange coefficient, k, greater than 7.5 x 10^-4 cm/s, …

Ethane Dehydrogenation For Light Olefins Production Over Stable Catalyst, Xiaoyan Wang

Graduate Theses, Dissertations, and Problem Reports (ETD)

Accompanied by the development of modern industry, the demand for light olefins (e.g., ethylene, propylene, butene, butadiene) increases year by year. Light olefins are important intermediates in producing polymers (Polyethylene, Polypropylene, etc.) and rubber (Styrene Butadiene Rubber, Polybutadiene rubber, etc.). The primary process for the production of light olefins is steam cracking of petroleum liquids (naphtha and distillate fuel oil). It is an energy-intensive process, requiring high temperature (750-850℃) and pressure (1.0-4.5 MPa). Meanwhile, due to undesired side reactions, this process has lowered the efficiency of light olefins production and suffers from severe coking issues. Furthermore, as petroleum liquids become …

Microwave-Assisted Carbon Nanotube Growth From Methane On Surface Catalyst Exsolving Perovskite Oxide, Angela M. Deibel

Graduate Theses, Dissertations, and Problem Reports (ETD)

The novel method of using a perovskite exsolution catalyst, strontium titanium nickel oxide (STNO), proved capable of simultaneously producing carbon nanotubes (CNTs) and CO_x-free hydrogen during methane decomposition under microwave irradiation. An optimization of common perovskite materials was conducted for microwave-responsiveness with the results reported in this study. Out of the materials screened, strontium titanium nickel oxide (STNO) was the best candidate to achieve an acceptable methane conversion rate as well as a decent responsiveness to microwave. STNO was further optimized through Ni content, reduction dwell time, and reduction temperature to produce the best methane conversion and CNT …

Dry Reforming Of Methane Using Microwave Irradiated Metal Oxide/Coal Char Catalysts, Anthony Carter

Graduate Theses, Dissertations, and Problem Reports (ETD)

This research focuses on the synthesis of both shaped and amorphous powder materials, the combination of these materials with dried Powder River Basin (PRB) coal char, and their reactionary properties with methane and carbon dioxide gasses with conventional and microwave (MW) heating. The first goal of this project was to synthesize shaped micro and nano sized particles with ideal dielectric properties for converting electromagnetic energy into heat and proven capabilities of activating methane. These particles were synthesized via solvothermal, hydrothermal, and co-preceptory treatments alone and onto the surface of dried PRB coal char. PRB is a sub-bituminous, low-ranking coal (LRC) …

Improving Performance And Durability Of Intermediate Temperature Proton‐Conducting Solid Oxide Electrolysis Cells Via Materials Design And Catalyst Surface Engineering, Hanchen Tian

Graduate Theses, Dissertations, and Problem Reports (ETD)

Solid oxide steam electrolysis cell, a promising electrical-chemical conversion device for the next generation efficient hydrogen production and energy storage, has been actively studied because of their high energy conversion efficiencies and prospective applications as electrochemical reactors. After decades of research on protonic ceramic materials, remarkable advances have been made in the protonic ceramic electrochemical cells (PCECs) air electrode and electrolyte. However, the existing air electrodes are far from satisfying the requirements of practical applications, a series of issues, including the lack of active and durable electrodes, greatly limit the commercialization. To date, the systematic development of triple conducting catalysts …

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. …

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 …

Valorization Of Xylan In Agroforestry Waste Streams, Harrison Appiah

Graduate Theses, Dissertations, and Problem Reports (ETD)

Valorization of Xylan in Agroforestry Waste Streams.

Harrison Appiah

Microwave-assisted deep eutectic solvent and gamma-valerolactone metallic chloride catalyzed conversion of xylan to furfural were investigated using a 2x3 factorial experimental design at two levels of percent microwave power, reaction time, and catalyst concentration. The levels of each factor studied were (20%, 60% microwave power, 2, 4 minutes, and 10, 20mg) respectively. The effect of three metallic chloride catalysts (LiCl, FeCl3.6H20, CuCl2) on the conversion of xylan to furfural was also investigated. The gamma-valerolactone-ferric chloride sent system exhibited the highest mean yield of furfural (56.50%). The next highest furfural yield of …

Natural Gas Conversion To Value-Added Chemicals By Microwave Catalytic Processes, Brandon Robinson

Graduate Theses, Dissertations, and Problem Reports (ETD)

Ethane is the second-largest component in natural gas and is typically separated out to minimize condensation in the pipelines. The technical difficulties and cost associated with the transportation and the storage of ethane have led companies to start burning natural gas to produce power or flaring which attributes to the global CO₂ emission problem. The conversion of ethane to higher-value liquid products is of increasing importance so that the natural gas can be safely utilized and cost-effectively transported. Existing commercial technologies used to convert ethane to liquid chemical products are typically based on the indirect syngas route, such as …

Biological Conversion Of Carbon Dioxide To Value-Added Chemicals, Owen James Mcgrath

Graduate Theses, Dissertations, and Problem Reports (ETD)

As Carbon Dioxide (CO₂) levels in the atmosphere continue to rise due to human intervention, there is increased urgency to take actions to mitigate the potential ramifications. Many countries have instituted a CO₂ tax and have provided funding to finding potential solutions to our growing CO₂ problem. Further investigating CO₂ capture, sequestration, and utilization is key to combating rising CO₂ levels and methods being investigated have increased substantially in recent years. Converting CO₂ into fuels and value-added chemicals provides a unique opportunity to create materials of value from a substance that is being …

Review Of Established And Emergent Methods For The Production Of C4 Olefins, James Matthew Koval

Graduate Theses, Dissertations, and Problem Reports (ETD)

Current production of C₄ olefins is dominated by naphtha cracking and butane dehydrogenation, but significant research interest is developing in alternate feedstocks due to an abundance of inexpensive natural gas and bioethanol. The current C₄ olefin production methods are costly, make use of already-depleted petroleum resources, and are often hazardous to workers, which forms the impetus for investigation into alternative methods and assessment of their viability as a future means of olefin production. Methods of natural gas conversion to higher order hydrocarbons are discussed, including Fischer-Tropsch synthesis and oxidative methane coupling, each of which could form the first …

Process Development Of Shale Gas Assisted Lignin And Biomass Reforming Through Novel Reaction Pathway And Catalyst Design To Produce Hydrogen Rich Syngas For Fuels And Value Added Chemicals, Amoolya D. Lalsare

Graduate Theses, Dissertations, and Problem Reports (ETD)

Novel biomass reforming strategy through synergistic co-processing with flare gas (methane and carbon dioxide) was developed at West Virginia University. Hardwood biomass comprised of lignin, hemicellulose, and cellulose is abundant in the US and potentially a sustainable source of hydrogen through extensive reforming and gasification. Ever-increasing shale gas production in the US occasionally leads to flaring owing to stranded production across the US. Achieving biomass co-processing with natural gas about to be flared in such stranded shale plays is the underlying motivation here. A novel reaction pathway was discovered wherein methane and carbon dioxide assisted reforming of biomass could be …

Cu-Based Electrocatalysts For Carbon Dioxide Conversion To Value-Added Chemicals, Qingyang Li

Graduate Theses, Dissertations, and Problem Reports (ETD)

Massive usage of fossil fuel has being causing considerable emission of CO₂, which increases the temperature of the planet and greatly threaten human living environment, such as soil degradation, lower agricultural productivity, desertification, less biodiversity, fresh-water reduction, ocean acidification, ozone sphere destruction, etc. A number of technologies are being developed to reduce the CO₂ amount, however, all existing technologies except utilizing CO₂ as a feedstock, are hardly to essentially close the anthropogenic carbon loop. Currently, considering the economy and operability, electroreduction of CO₂ seems to be the most promising strategy to convert CO₂ to …

Process Modeling And Techno-Economic Analysis Of Thermo-Catalytic Dimethyl Ether Synthesis And Microwave-Based Aromatics Production Technologies From Shale Gas, Chirag Mevawala

Graduate Theses, Dissertations, and Problem Reports (ETD)

Production of dimethyl ether (DME) and direct non-oxidative methane dehydroaromatization (DHA) to aromatics via conventional and microwave (MW)-assisted processes are investigated in this research. Plant-wide models of the shale gas to DME process with integrated CO₂ capture via direct and indirect synthesis routes have been developed. Optimal parameter estimation, and model validation are undertaken for various sections of the process including the pre-reforming reactor, auto-thermal reforming reactor, DME synthesis reactors, CO₂ capture units and separation sections. A novel DME separation process has been developed for efficient separation of DME, syngas, and CO₂. Plant-wide techno-economic optimization is …

Dynamic Study Of Mo/Zsm-5 Catalyst For Ch4 Dehydroadomation, Hadi Yahya Almusawa

Graduate Theses, Dissertations, and Problem Reports (ETD)

Methane dehydroaromatization (CH₄-MDA) is a highly promising venture for natural gas utilization/exploitation, i.e., direct conversion of methane (CH₄) to liquid aromatics (benzene) and hydrogen. This process is a catalytic reaction and therefore, is subject to all the advantages and constraints of catalysis. This study discussed the structure and reactivity of Mo/ZSM-5 zeolite catalysts and their effect on the active conversion of methane to valuable aromatic products such as benzene: 1) The preparation and characterization of Mo/ZSM-5, which are crucial steps in any catalytic reaction process since a better performing catalyst consequently leads to better outcomes; 2) …

Mechanism Study Of Shale Gas Conversion Via Chemical Looping And Heterocatalytic Processes, Lei Bai

Graduate Theses, Dissertations, and Problem Reports (ETD)

The shale gas revolution has significantly changed the energy landscape in US. The technical-feasible, energy-effective schemes for shale gas combustion and utilization, especially from remote resources, have attracted increasing interest due to expensive transportation/distribution cost. In this research, for the first time, chemical looping combustion (CLC) of methane with inherent CO₂ capture, oxidative coupling of methane (OCM) and dehydro-aromatization (DHA) of ethane are systematically studied as promising alternatives at O₂-rich, O₂-lean and non-oxidative conditions, respectively.

Chemical looping combustion is bridging clean fuel combustion in energy production with inherent CO₂ capture. CLC utilized an oxygen …