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Core-Shell Oxidative Aromatization Catalysts for Single Step Liquefaction of Distributed Shale Gas (Final Technical Report)
The objective of this project was to design and demonstrate a core-shell structured multifunctional catalyst to convert the light (dry) components of shale gas into liquid aromatic compounds (primarily benzene and toluene) in a single step. Operated in a modular oxidative aromatization system (OAS) under a cyclic redox scheme, the novel catalyst and process can significantly improve the value and transportability of distributed shale gas. Since the project started, each quarter addressed a different set of tasks related to the completion of the milestone detailed in the project award. The yearly summaries of these tasks are summarized below: Q1-Q4: • Conducted project planning and literature search. • Investigated a number of SHC redox catalysts using thermogravimetric analysis and fixed-bed reactor experiments. • Initiated process modeling towards generating two process models for the methane DHA base case and OAS process. • Developed DHA catalysts capable of producing >500 g/kg-cat-hr aromatics at 80% or greater aromatics selectivity at 700°C. Q5-Q8: • Developed alternative approaches with sequential bed configurations to enhance the aromatic yields based on OCM+DHA • Improved the zeolite synthesis efficiency by using the microwave-assisted technique and investigated the synthesis conditions on the zeolite yield, crystalline structure and morphology • Constructed a set of Aspen Plus process models with significant energy savings for OAS as compared to the base case non-oxidative DHA. • Adapted conventional hydrothermal method to be applicable to the microwave synthesizer unit for more efficient catalyst synthesis. • Studied the structure of the OCM catalyst and the dispersion of the carbonate in the redox reactions and in methane flow with Raman Spectroscopy. Q9-Q12: • Scaled up the catalyst synthesis with the microwave synthesis method. Based on its performance, procedural characterizations and catalytic performance testing were further conducted for the new microwave synthesized catalysts with the newly-developed product analysis procedure. • Developed the reaction system setup for the C2-DHA or OCM+DHA reaction product and achieved a better product collection-analysis method for the aromatic products with an improved carbon balance. The product from the OCM reaction exhibited complicated effects on the DHA catalyst. • Conducted additional OCM catalyst characterization using Near Ambient Pressure X-ray Photoelectron Spectroscopy and in situ Raman characterization • Validated the significant energy savings for OAS as compared to the base case non-oxidative DHA. Successfully set up the simulation model for the OCM+DHA+SHC reaction system based on the updated experimental results from NCSU. Q13-End of project: • Synthesized new zeolite catalysts by the microwave method, conducted characterizations (XRD, SEM, and TEM) and catalytic behavior testing. • Explored the “wet” C 2 H 6 and C 2 H 4 DHA reactions with using steam co-feed. A subsequent reduction as the regeneration step can regenerate the DHA catalyst and recover 99% activity of the fresh performance. • Achieved a 15.3% single-pass aromatic yield from methane by rationally combining the OCM and DHA at different temperatures. • Conducted a 105-hour stability test with an improved regeneration procedure, with an average aromatic yield of 13.8%. • Developed new catalyst and achieved a record-high 23.2% yield.
Liquefaction dynamics of n-octadecane in cylindrical coordinates
The study presents one method of mathematically modeling the effects of gravity-induced free convection upon the melting phenomena of a finite paraffin slab. The theoretical model is based on the numerical computer solution of the solid phase and liquid phase energy equations, coupled with an imposed ideal-viscous flow approximation. An implicit alternating-direction technique is used as the finite-difference approximation for the basic energy equations in the numerical solution. The theoretical predictions are compared to experimental data from an annular test cell, in which n-octadecane, C18H38, was used as the test material. The results show that the model is a good first approximation to the solution of solid-liquid phase change involving gravity-induced free convection.
Coal liquefaction to increase jet fuel production
Processing concept that increases supply of jet fuel has been developed as part of study on methods for converting coal to hydrogen, methane, and jet fuel. Concept takes advantage of high aromatic content of coal-derived liquids to make high-octane gasoline, instead of destroying aromatics to make jet fuel.
One-Step Coal Liquefaction
Steam injection improves yield and quality of product. Single step process for liquefying coal increases liquid yield and reduces hydrogen consumption. Principal difference between this and earlier processes includes injection of steam into reactor. Steam lowers viscosity of liquid product, so further upgrading unnecessary.
Catalytic Coal Liquefaction With Iron Sulfate
Very high conversion yields demonstrated with iron sulfate used in solution with water or solvent to impregnate coal.
Prospects for utilization of air liquefaction and enrichment system (ALES) propulsion in fully reusable launch vehicles
A concept is shown for a fully reusable, earth to orbit launch vehicle with horizontal takeoff and landing, employing an air-turborocket for low speed and a rocket for high speed acceleration, both using LH2 fuel. The turborocket employs a modified liquid air cycle to supply the oxidizer. The rocket uses 90 percent pure LOX that is collected from the atmosphere, separated, and stored during operation of the turborocket from about Mach 2 to Mach 5 or 6. The takeoff weight and the thrust required at takeoff are markedly reduced by collecting the rocket oxidizer in-flight. The paper shows an approach and the corresponding technology needs for using ALES propulsion in a SSTO vehicle. Reducing the trajectory altitude at the end of collection reduces the wing area and increases payload. The use of state-of-the-art materials, such as graphite polyimide, is critical to meet the structure weight objective for SSTO. Configurations that utilize 'waverider' aerodynamics show great promise to reduce the vehicle weight.
Liquefaction of Air in the Langley 11-inch Hypersonic Tunnel
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Oxygen liquefaction and zero-loss storage system
This paper presents an alternative concept that employs existing technologies and off-the-shelf components to liquefy gaseous oxygen from an in-situ propellant production (ISPP) unit and to store the liquid oxygen without boil-off loss. A primary goal is to minimize active components with a secondary goal of designing the active component in a protected or failure-free environment. The resulting design requires only one active component, a compressor operating in a closed and consequently more protected system. The design avoids pumps as active components by employing cryopumping for gaseous oxygen (GOX) and gravity transfer for liquid oxygen (LOX).
Cryogenic Fluid In-Situ Liquefaction for Landers "Brassboard" Overview
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C3Or3C-02: In-situ, High-spatial Resolution Temperature Measurement of Liquid Oxygen Tank under Liquefaction via Fiber Optics Sensing System
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Hydrothermal Liquefaction of Food Waste and Remediation of Aqueous Byproducts
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Advanced multi-layer active magnetic regenerator systems and processes for magnetocaloric liquefaction
A process for liquefying a process gas that includes introducing a heat transfer fluid into an active magnetic regenerative refrigerator apparatus that comprises a single stage comprising dual multilayer regenerators located axially opposite to each other.
Advanced multi-layer active magnetic regenerator systems and processes for magnetocaloric liquefaction
A process for liquefying a process gas that includes introducing a heat transfer fluid into an active magnetic regenerative refrigerator apparatus that comprises a single stage comprising dual multilayer regenerators located axially opposite to each other.
Co-Processing Fast Pyrolysis Bio-Oils and Hydrothermal Liquefaction Biocrudes in Fluid Catalytic Cracking and Hydroprocessing in Refineries
Co-processing of biogenic feedstocks within the existing petroleum infrastructure represents an opportunity to incorporate large volumes of bio-carbon into transportation fuels. However, upgrading intermediate liquids from biomass and waste to final products efficiently and economically, while minimizing impacts to existing refinery infrastructure, remains a notable barrier to commercialization. The co-processing project, Bio-oil Co-processing with Refinery Streams, aimed to generate foundational knowledge for processing renewable intermediates in petroleum refineries and offer co-processing strategies, as well as develop new methods for biogenic carbon tracking and measurement.