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Siriwardane, Ranjani

Publications and source records attributed to Siriwardane, Ranjani.

At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Towards a standard approach to the analysis of carbon products generated from Natural Gas pyrolysis

Conference presentation for the work entitled “A standard approach to the analysis of carbon products generated from Natural Gas pyrolysis”. Pyrolysis of natural gas (NGP) has been proposed as a near term solution for the production of direct CO2 free (turquoise) hydrogen, to help fuel a more sustainable energy future. NGP can serve as a bridging technology while other (green) hydrogen production technologies mature. In order for NGP to be successful, the management of the generated carbon products needs to be carefully considered. Necessary markets need to be considered to incorporate the (turquoise) carbon products that are generated. A large hurdle in addressing the channeling of carbon products into desired markets is determining exactly what is manufactured from the NGP process. In this work an analysis method is presented that combines a suite of techniques for the assessment of the carbon product from Natural Gas Pyrolysis for appropriate identification and quality control.

Riley, Jarrett↗
DOE OSTI2024

Advanced Reaction Systems

An overview of NETL's Gasification Systems R&D was provided at DOE's Hydrogen and Fuel Cells Technology Office (HFTO) Annual Merit Review (AMR) on May 7, 2024, in Arlington, VA. The objective of the Advanced Reaction Systems Portfolio is to design, develop, and analyze technologies to support the mission of the Gasification Program to enable the use of diverse feedstocks to produce hydrogen and other value-added products with net-zero greenhouse gas emissions.

Lewis, Eric↗
DOE OSTI2024

Advanced Reaction Systems

An overview of NETL's Gasification Systems R&D was provided at the 2024 FECM/NETL Spring R&D Project Review Meeting on April 24, 2024, in Pittsburgh, PA. The objective of the Advanced Reaction Systems Portfolio is to design, develop, and analyze technologies to support the mission of the Gasification Program to enable the use of diverse feedstocks to produce hydrogen and other value-added products with net-zero greenhouse gas emissions.

Lewis, Eric↗
DOE OSTI2023

TGA Study of the Reaction Kinetics of a CuFeMnAlO 4+δ Oxygen Carrier for Methane Chemical Looping Combustion under High Pressure and Atmospheric Pressure Conditions

Reduction and oxidation kinetics of a CuFeMnAlO 4+δ oxygen carrier for methane were studied using an atmospheric thermogravimetric analyzer (TGA) and a pressurized TGA. Important parameters such as temperature (500–900 °C), particle size distribution (150–650 μm), and partial pressures of reactants (methane and oxygen) were evaluated. Results showed that the reduction of the oxygen carrier was not affected by particle size distribution studied in this work, and that above 750 °C, the effect of the temperature on oxygen carrier reduction started to diminish. The reaction time approaches an asymptotic limit as methane partial pressure increases. For oxygen carrier oxidation, it was found that the rate of oxidation increased with increasing oxygen concentration. The effect of the oxygen concentration was more noticeable when the oxygen concentration was below 7.5%. Because of the inherent feature of the oxygen carrier, its chemical looping with oxygen uncoupling property was also assessed. A phase boundary-controlled shrinking sphere model was used to model the test data from the TGAs. Modeling results showed that the oxygen carrier reduction had a reaction order of 1 with an activation energy of ∼46 kJ/mol. Oxygen carrier oxidation demonstrated a reaction order of 1.1 with an activation energy of ∼55 kJ/mol. Additionally, the differences of the experimental results between the atmospheric pressure TGA and the pressurized TGA were discussed in detail and the limitations of the pressurized TGA were highlighted.

Hydrocarbons↗
DOE OSTI2023

Investigation of methane and ethane pyrolysis with highly active and durable iron-alumina catalyst to produce hydrogen and valuable nano carbons: Continuous fluidized bed tests and reaction rate analysis

The goal of this research work was to evaluate a novel iron-alumina catalyst for methane and ethane pyrolysis with high conversion rates to H 2 with a long life time to address two major issues reported with previous catalysts. Fluidized bed tests demonstrated continuous hydrogen production while collecting carbon containing fines. During the 230 h fluid bed test the methane conversion rate to hydrogen at 700 °C remained above 80% for 160 h while creating valuable nano carbons. Similarly high catalyst lifetimes with high methane conversions have not been reported before. Ethane was more active than methane for pyrolysis with 100% conversion to H 2 . Transmission electron microscopy and Raman analysis of the carbon showed single and multiwall nanotubes and conglomerate nano-fibers. Ethane did not impact the allotrope of carbon formed. TGA was used to create a data array that was used for kinetic analysis and reaction model parametric regressions. Ethane had a higher rate of pyrolysis that was 2.3–2.8 times that of methane. Ethane pyrolysis was found to be more sensitive to temperature with a higher activation energy of 62 kJ/mol as compared to methane at 43 kJ/mol. The frequency factor, A i , was significantly higher for ethane at 0.73 [[kmol/m 3 -sec]/[N/m2] n ] compared to 0.03 for methane on the same basis. Both gases had a functional partial pressure order dependence of ~0.6 based on the regression analysis.

08 HYDROGEN↗
DOE OSTI2022

Encapsulation method for preparation of pellets with high attrition resistance

This disclosure provides a method to produce highly attrition resistant pellets by encapsulating reactive components in a vitrified clay outer layer. The reactive component mixture is present relative to the clay substrate in a weight ratio of part per 60-100 part to about 60 parts of the clay substrate. The reactive components are agglomerated first, and clay substrate is added to form the outer layer of the pellet. The pellets are calcined at temperatures above 1200 C to form a vitrified clay semi porous outer layer providing high strength to the pellet while facilitating the gas transfer for the reaction with the encapsulated reactive components. Pellets containing CuO—Fe 2 O 3 -alumina oxygen carrier for chemical looping combustion of fuel demonstrated high attrition resistance and high reactivity with methane.

Siriwardane, Ranjani↗
DOE OSTI2022

Iron based catalysts for production of carbon and hydrogen from decomposition of methane

The invention provides a calcined Fe x —Al y —O z based catalyst for the decomposition of hydrocarbons such as methane to produce hydrogen and carbon. The catalyst comprises iron oxide mixed with aluminum oxide and calcined at temperatures above 1100° C., where Fe x —Al y —O z is a chemical composition with x>0.1, y>0.1, z≥0 and 0 2 and carbon. In an embodiment, carbon is separated from the catalyst and the catalyst is reused for continuous methane decomposition to produce H 2 .

Siriwardane, Ranjani↗
DOE OSTI2022

CO 2 utilization potential of a novel calcium ferrite based looping process fueled with coal: Experimental evaluation of various coal feedstocks and thermodynamic integrated process analysis

Here, conversion of CO 2 to CO was performed at 800-850C via reduction of calcium ferrite (CaFe 2 O 4 ) with coal followed by oxidation of reduced CaFe 2 O 4 with CO 2 to produce CO and partially oxidized Ca ferrite. The process was evaluated with several types of coals which included lignite, sub-bituminous, bituminous, anthracite and pet-coke. Reduction of CaFe 2 O 4 with sub-bituminous coal and lignite coal was more favorable than that with higher rank coals. Stable reactivity performance was demonstrated for 35-cycle test conducted with lignite coal/CaFe 2 O 4 at 800°C and with high conversion of CO 2 to CO. The rate of conversion of CO 2 to CO with reduced CaFe 2 O 4 was found to be 1st order with respect to CO 2 and had a low activation energy of 7.4 kJ/mol. Thermodynamic integrated process assessments suggest that two and three reactor process concepts can be realized and net CO 2 utilization achievable. The two reactor configuration shows the highest potential for CO 2 utilization while generating a value-added CO rich syngas stream.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Cooperative Research and Development Agreement between National Energy Technology Laboratory and Birla Carbon U.S.A., Inc. [Final Report]

NETL researchers collaborated with Birla Carbon, U.S.A., to leverage NETL's patented catalyst work on methane decomposition to develop a cost-effective process for production of hydrogen and valuable carbon from natural gas. This process is cost-effective, energy efficient and environmentally friendly with minimal CO 2 mitigation costs. The objectives of the project include evaluation of effect of feed gas composition of natural gas on the performance, lowering the catalyst production cost and to conduct cost analysis for a process.

03 NATURAL GAS↗
DOE OSTI2021

Development of CuFeMnAlO 4+δ oxygen carrier with high attrition resistance and 50-kWth methane/air chemical looping combustion tests

A Copper-Ferri-Manganese-Aluminate spinel (CuFeMnAlO 4+δ ) oxygen carrier, developed at the US Department of Energy’s (DOE) National Energy Technology Laboratory (NETL), shows promising results for chemical looping combustion with methane. Attrition resistance of the spinel oxygen carrier (160–600 µm) produced by a wet agglomeration method was significantly higher than that observed previously with a Copper-Ferri-Aluminate (CuFeAlO 4 ) oxygen carrier. Improved attrition resistance of the novel carrier can be attributed to minimal alumina phase segregation and minimal carbon formation. Heats of reaction measured by differential scanning calorimetry indicated exothermicity during reduction with methane. The total oxygen transfer capacity of the material was about 10.5 wt% at 850 °C. The attrition resistance and the oxygen transfer capacity of the carrier prepared at a commercial manufacturing facility (180 kg) were very similar to observed values during the development phase with the lab scale preparations. The material displays satisfactory methane conversion and significantly high particle durability during a 54 h test campaign conducted in NETL’s 50-kWth chemical looping dual fluid bed reactor unit at temperatures ranging from 700 to 900 °C. Low oxygen carrier make-up cost, due to the use of natural ore and pigment grade raw materials during synthesis and very low attrition rates, exceeded the performance goals determined by systems studies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Particle-Scale Reduction Analysis of CuFeMnO 4 with Hydrogen for Chemical Looping Combustion

In this work CuFeMnO 4 (copper iron manganese oxide) oxygen carrier was characterized using DSC/TGA, in-situ XRD, and SEM-EDS to gain a clear elucidation of the chemical looping combustion (CLC) reactions with H2 which is a component of synthesis gas. A reaction model which best described the experimental TGA reaction data was selected from the analysis. Intrinsic rate of reaction parameters obtained from the study could be used for designing a reactor for scale-up. A model with combined contributions from nucleation and growth model and dimensional phase boundary model was found to exhibit the best correlation with the experimental data. The analysis provided validation of intrinsic reaction rates and other rate parameters.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Cooperative Research and Development Agreement between National Energy Technology Laboratory and Birla Carbon U.S.A., Inc. [Abstract]

NETL researchers will be collaborating with Birla Carbon, U.S.A., Inc. (Birla Carbon) to leverage NETL's patented catalyst work on methane decomposition to commercialize an efficient and a cost-effective process for production of hydrogen and valuable carbon from natural gas. This catalytic methane decomposition is a promising technology, however, finding an appropriate catalyst to perform all the functions has been a challenge. NETL has developed a suitable catalyst for the process which has shown promising results. The heat required for this endothermic catalytic decomposition process is provided by combustion of a portion of the hydrogen. This process is cost effective, energy efficient, and environmentally friendly with minimal CO 2 mitigation costs. The objectives of the project include evaluation of the effect of feed gas composition on the performance, reduction of the catalyst production cost, and conduction of an in-depth large-scale cost analysis for a process suitable for applications at Birla Carbon.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Interaction of Methane with Calcium Ferrite in the Chemical Looping Partial Oxidation Application: Experimental and DFT Study

In this study, experimental studies using mass spectroscopy, thermogravimetric analysis, in situ X-ray diffraction (XRD), and theoretical density functional theory calculations were carried out to investigate the mechanism of methane partial oxidation over a CaFe 2 O 4 oxygen carrier. The XRD analysis revealed the formation of the calcium ferrite phases during methane reduction occurred in the sequence CaFe 2 O 4 →CaFe 3 O 5 + Ca 2 Fe 2 O 5 →FeO + Fe + CaO→Fe + CaO. Each of these phases was modeled using periodic density functional theory to study the activity of these phases for the reactivity with CH 4 , CO, and H 2 along with the adsorbed surface species to help elucidate the effect that phase changes during reduction have on the chemical looping products CO and H 2 . Mass spectroscopic analysis revealed the formation of H 2 O and CO 2 occurred prior to the formation of CO and H 2 , and these products may be due to the removal of lattice oxygen bound in the discrete primary phase, which contributes to a small portion (~16%) of the total transferable oxygen in the solid. The density functional theory (DFT) results suggest that the gaseous CO and H 2 are not thermodynamically favorable to react with the Ca 2 Fe 2 O 5 where the release of CO and H 2 led to an increase in selectivity for these products. The DFT results suggest that some of the adsorbed atomic hydrogen combined to form adsorbed H 2 and then gaseous H 2 on the CaFe 2 O 4 surface, while the carbon deposition and some adsorbed atomic hydrogen react to form the CaFe 3 O 5 and Ca 2 Fe 2 O 5 phases simultaneously. DFT simulations suggest that both the gaseous H 2 and adsorbed atomic H are less thermodynamically favorable to drive the deep reduction of Ca 2 Fe 2 O 5 to CaO and Fe0. The deep reduction of the calcium ferrite therefore favors the generation of syngas products (CO and H 2 ) through mechanisms of methane dehydrogenation and selective oxidation of carbon to CO. The significant difference in mechanisms for partial oxidation of methane to syngas with the CaFe 2 O 4 carrier can be correlated to the differences in the oxide phases present during the reduction process, concentration of oxygen species, and bonding in the lattice structure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗