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Robert James Perry - One of the best experts on this subject based on the ideXlab platform.
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Measurement of CO2 Diffusivity in Phase-Changing Aminosilicone CO2 Capture Solvent
Energy & Fuels, 2018Co-Authors: Tiffany Elizabeth Pinard Westendorf, Benjamin Rue Wood, Robert James Perry, Rachel L Farnum, Robert M Enick, Gosia Rubinsztajn, John Brian Mcdermott, Deepak TapriyalAbstract:The mass transfer performance of a phase-changing aminosilicone CO2 post-combustion capture absorbent has been characterized. The aminosilicone, 1,3-bis(3-aminopropyl)-1,1,3,3-tetramethyldisiloxane (GAP-0), rapidly transforms from a low-viscosity liquid into a friable solid upon exposure to gaseous CO2. Mass transfer performance of this absorbent was studied to inform design and scaleup of a CO2 capture process. The long-term mass transfer rate of CO2 gas through a solid GAP-0 carbamate salt layer into a quiescent pool of liquid GAP-0 was characterized using pressurized thermogravimetric analysis. This experiment led to an estimate of the CO2 permeability of the carbamate salt solid of 1.46 × 10–9 mol of CO2 m–1 s–1 atm–1. Given literature-reported values of CO2 solubility in silicone polymers, the CO2 diffusivity through GAP-0 carbamate salt was inferred to be approximately 4.39 × 10–11 m2/s. In parallel, the CO2 absorption rate into a spray of GAP-0 droplets was studied in a laboratory spray reactor. Wh...
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second generation Aminosilicones as co2 capture solvents
Energy & Fuels, 2017Co-Authors: Robert James PerryAbstract:Silicones with a variety of linear, branched, star, and cyclic architectures were synthesized that contained electron-donating ethylaminopropyl groups attached to the silicone core. These solvents were tested for CO2 uptake and their physical state after reaction. In comparison to analogous materials that only possessed a primary amine, all of the heteroatom-substituted derivatives displayed excellent CO2 uptake and all maintained a liquid, flowable state after reaction. Optimal CO2 uptake was achieved at ambient temperatures rather than the typical 40 °C level. This was likely due to the lower heats of reaction for the secondary amine structure. β-Isomer present in the samples did not adversely affect the reaction with CO2 or the ability to remain in a liquid state upon complete reaction.
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Measuring CO2 and N2O Mass Transfer into GAP-1 CO2–Capture Solvents at Varied Water Loadings
Industrial & Engineering Chemistry Research, 2017Co-Authors: Greg A. Whyatt, Irina Spiry, Benjamin Rue Wood, Robert James Perry, Andy Zwoster, Feng Zheng, Charles J. Freeman, David J. HeldebrantAbstract:This paper investigates the CO2 and N2O absorption behavior in the water-lean gamma amino propyl (GAP)-1/TEG solvent system using a wetted-wall contactor. Testing was performed on a blend of GAP-1 aminosilicone in triethylene glycol at varied water loadings in the solvent. Measurements were made with CO2 and N2O at representative lean (0.04 mol CO2/mol alkalinity), middle (0.13 mol CO2/mol alkalinity), and rich (0.46 mol CO2/mol alkalinity) solvent loadings at 0, 5, 10, and 15 wt % water loadings at 40, 60, and 80 °C and N2O at (0.08–0.09 mol CO2/mol alkalinity) at 5 wt % water at 40, 60, and 80 °C. CO2 flux was found to be nonlinear with respect to log mean pressure driving force (LMPD). Liquid-film mass transfer coefficients (k′g) were calculated by subtracting the gas film resistance (determined from a correlation from literature) from the overall mass transfer measurement. The resulting k′g values for CO2 and N2O in GAP-1/TEG mixtures were found to be higher than that of 5 M aqueous monoethanolamine u...
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Thermal Degradation of Aminosilicone Carbamates
Energy & Fuels, 2016Co-Authors: Robert James Perry, Benjamin Rue Wood, Matthew P. Rainka, Mark D. Doherty, Omkar Namjoshi, Daniel Hatchell, Gary T. RochelleAbstract:The major thermal degradation pathway seen with 1,5-bis(3-aminopropyl)-1,1,3,3,5,5-hexamethyltrisiloxane/triethylene glycol (GAP-1/TEG) is the formation of a urea-containing compound. Degradation is increased at higher temperatures, longer reaction times, higher CO2 concentrations (in the form of carbamate loading), and low water levels. A judicious choice of operating conditions can significantly decrease urea byproduct formation. Reducing the desorption temperature from 140 to 100 °C and adding 5 wt % water to the 60:40 mixture of GAP-1/TEG resulted in a 500-fold reduction in amine loss after 4 days in a CO2-rich environment. After 56 days of continuous heating under the same conditions, ∼87% original GAP-1 was retained at 100 °C compared to only ∼20% at 140 °C. The urea byproduct appears to be the only major degradation pathway under these conditions, with 100% of the mass balance accounted for by the urea and amine components.
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Bench-Scale Process for Low-Cost Carbon Dioxide (CO2) Capture Using a Phase-Changing Absorbent
2015Co-Authors: Tiffany Elizabeth Pinard Westendorf, Irina Spiry, Robert James Perry, Joel Caraher, Wei Chen, Rachael Farnum, Paul Wilson, Benjamin Rue WoodAbstract:The objective of this project is to design and build a bench-scale process for a novel phase-changing aminosilicone-based CO2-capture solvent. The project will establish scalability and technical and economic feasibility of using a phase-changing CO2-capture absorbent for post-combustion capture of CO2 from coal-fired power plants with 90% capture efficiency and 95% CO2 purity at a cost of $40/tonne of CO2 captured by 2025 and a cost of
Benjamin Rue Wood - One of the best experts on this subject based on the ideXlab platform.
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Measurement of CO2 Diffusivity in Phase-Changing Aminosilicone CO2 Capture Solvent
Energy & Fuels, 2018Co-Authors: Tiffany Elizabeth Pinard Westendorf, Benjamin Rue Wood, Robert James Perry, Rachel L Farnum, Robert M Enick, Gosia Rubinsztajn, John Brian Mcdermott, Deepak TapriyalAbstract:The mass transfer performance of a phase-changing aminosilicone CO2 post-combustion capture absorbent has been characterized. The aminosilicone, 1,3-bis(3-aminopropyl)-1,1,3,3-tetramethyldisiloxane (GAP-0), rapidly transforms from a low-viscosity liquid into a friable solid upon exposure to gaseous CO2. Mass transfer performance of this absorbent was studied to inform design and scaleup of a CO2 capture process. The long-term mass transfer rate of CO2 gas through a solid GAP-0 carbamate salt layer into a quiescent pool of liquid GAP-0 was characterized using pressurized thermogravimetric analysis. This experiment led to an estimate of the CO2 permeability of the carbamate salt solid of 1.46 × 10–9 mol of CO2 m–1 s–1 atm–1. Given literature-reported values of CO2 solubility in silicone polymers, the CO2 diffusivity through GAP-0 carbamate salt was inferred to be approximately 4.39 × 10–11 m2/s. In parallel, the CO2 absorption rate into a spray of GAP-0 droplets was studied in a laboratory spray reactor. Wh...
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Measuring CO2 and N2O Mass Transfer into GAP-1 CO2–Capture Solvents at Varied Water Loadings
Industrial & Engineering Chemistry Research, 2017Co-Authors: Greg A. Whyatt, Irina Spiry, Benjamin Rue Wood, Robert James Perry, Andy Zwoster, Feng Zheng, Charles J. Freeman, David J. HeldebrantAbstract:This paper investigates the CO2 and N2O absorption behavior in the water-lean gamma amino propyl (GAP)-1/TEG solvent system using a wetted-wall contactor. Testing was performed on a blend of GAP-1 aminosilicone in triethylene glycol at varied water loadings in the solvent. Measurements were made with CO2 and N2O at representative lean (0.04 mol CO2/mol alkalinity), middle (0.13 mol CO2/mol alkalinity), and rich (0.46 mol CO2/mol alkalinity) solvent loadings at 0, 5, 10, and 15 wt % water loadings at 40, 60, and 80 °C and N2O at (0.08–0.09 mol CO2/mol alkalinity) at 5 wt % water at 40, 60, and 80 °C. CO2 flux was found to be nonlinear with respect to log mean pressure driving force (LMPD). Liquid-film mass transfer coefficients (k′g) were calculated by subtracting the gas film resistance (determined from a correlation from literature) from the overall mass transfer measurement. The resulting k′g values for CO2 and N2O in GAP-1/TEG mixtures were found to be higher than that of 5 M aqueous monoethanolamine u...
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Thermal Degradation of Aminosilicone Carbamates
Energy & Fuels, 2016Co-Authors: Robert James Perry, Benjamin Rue Wood, Matthew P. Rainka, Mark D. Doherty, Omkar Namjoshi, Daniel Hatchell, Gary T. RochelleAbstract:The major thermal degradation pathway seen with 1,5-bis(3-aminopropyl)-1,1,3,3,5,5-hexamethyltrisiloxane/triethylene glycol (GAP-1/TEG) is the formation of a urea-containing compound. Degradation is increased at higher temperatures, longer reaction times, higher CO2 concentrations (in the form of carbamate loading), and low water levels. A judicious choice of operating conditions can significantly decrease urea byproduct formation. Reducing the desorption temperature from 140 to 100 °C and adding 5 wt % water to the 60:40 mixture of GAP-1/TEG resulted in a 500-fold reduction in amine loss after 4 days in a CO2-rich environment. After 56 days of continuous heating under the same conditions, ∼87% original GAP-1 was retained at 100 °C compared to only ∼20% at 140 °C. The urea byproduct appears to be the only major degradation pathway under these conditions, with 100% of the mass balance accounted for by the urea and amine components.
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Bench-Scale Process for Low-Cost Carbon Dioxide (CO2) Capture Using a Phase-Changing Absorbent
2015Co-Authors: Tiffany Elizabeth Pinard Westendorf, Irina Spiry, Robert James Perry, Joel Caraher, Wei Chen, Rachael Farnum, Paul Wilson, Benjamin Rue WoodAbstract:The objective of this project is to design and build a bench-scale process for a novel phase-changing aminosilicone-based CO2-capture solvent. The project will establish scalability and technical and economic feasibility of using a phase-changing CO2-capture absorbent for post-combustion capture of CO2 from coal-fired power plants with 90% capture efficiency and 95% CO2 purity at a cost of $40/tonne of CO2 captured by 2025 and a cost of
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Pilot-Scale Silicone Process for Low-Cost Carbon Dioxide Capture
2014Co-Authors: Surinder Prabhjot Singh, Irina Spiry, Benjamin Rue Wood, Dan Hancu, Wei ChenAbstract:GE Global Research is developing technology to remove carbon dioxide (CO 2) from the flue gas of coal-fired powerplants. A mixture of 3-aminopropyl end-capped polydimethylsiloxane (GAP-1m) and triethylene glycol (TEG) is the preferred CO2-capture solvent. GE Global Research was contracted by the Department of Energy to test a pilot-scale continuous CO2 absorption/desorption system using a GAP-1m/TEG mixture as the solvent. As part of that effort, an Environmental, Health, and Safety (EH&S) assessment for a CO2-capture system for a 550 MW coal-fired powerplant was conducted. Five components of the solvent, CAS#2469-55-8 (GAP-0), CAS#106214-84-0 (GAP-1-4), TEG, and methanol and xylene (minor contaminants from the aminosilicone) are included in this assessment. One by-product, GAP- 1m/SOX salt, and dodecylbenzenesulfonicacid (DDBSA) were also identified foranalysis. An EH&S assessment was also completed for the manufacturing process for the GAP-1m solvent. The chemicals associated with the manufacturing process include methanol, xylene, allyl chloride, potassium cyanate, sodium hydroxide (NaOH), tetramethyldisiloxane (TMDSO), tetramethyl ammonium hydroxide, Karstedt catalyst, octamethylcyclotetrasiloxane (D4), Aliquat 336, methyl carbamate, potassium chloride, trimethylamine, and (3-aminopropyl) dimethyl silanol. The toxicological effects of each component of both the CO2 capture system and the manufacturing process were defined, and control mechanisms necessary to comply with U.S. EH&S regulations aremore » summarized. Engineering and control systems, including environmental abatement, are described for minimizing exposure and release of the chemical components. Proper handling and storage recommendations are made for each chemical to minimize risk to workers and the surrounding community.« less
Irina Spiry - One of the best experts on this subject based on the ideXlab platform.
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Measuring CO2 and N2O Mass Transfer into GAP-1 CO2–Capture Solvents at Varied Water Loadings
Industrial & Engineering Chemistry Research, 2017Co-Authors: Greg A. Whyatt, Irina Spiry, Benjamin Rue Wood, Robert James Perry, Andy Zwoster, Feng Zheng, Charles J. Freeman, David J. HeldebrantAbstract:This paper investigates the CO2 and N2O absorption behavior in the water-lean gamma amino propyl (GAP)-1/TEG solvent system using a wetted-wall contactor. Testing was performed on a blend of GAP-1 aminosilicone in triethylene glycol at varied water loadings in the solvent. Measurements were made with CO2 and N2O at representative lean (0.04 mol CO2/mol alkalinity), middle (0.13 mol CO2/mol alkalinity), and rich (0.46 mol CO2/mol alkalinity) solvent loadings at 0, 5, 10, and 15 wt % water loadings at 40, 60, and 80 °C and N2O at (0.08–0.09 mol CO2/mol alkalinity) at 5 wt % water at 40, 60, and 80 °C. CO2 flux was found to be nonlinear with respect to log mean pressure driving force (LMPD). Liquid-film mass transfer coefficients (k′g) were calculated by subtracting the gas film resistance (determined from a correlation from literature) from the overall mass transfer measurement. The resulting k′g values for CO2 and N2O in GAP-1/TEG mixtures were found to be higher than that of 5 M aqueous monoethanolamine u...
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Bench-Scale Process for Low-Cost Carbon Dioxide (CO2) Capture Using a Phase-Changing Absorbent
2015Co-Authors: Tiffany Elizabeth Pinard Westendorf, Irina Spiry, Robert James Perry, Joel Caraher, Wei Chen, Rachael Farnum, Paul Wilson, Benjamin Rue WoodAbstract:The objective of this project is to design and build a bench-scale process for a novel phase-changing aminosilicone-based CO2-capture solvent. The project will establish scalability and technical and economic feasibility of using a phase-changing CO2-capture absorbent for post-combustion capture of CO2 from coal-fired power plants with 90% capture efficiency and 95% CO2 purity at a cost of $40/tonne of CO2 captured by 2025 and a cost of
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Pilot-Scale Silicone Process for Low-Cost Carbon Dioxide Capture
2014Co-Authors: Surinder Prabhjot Singh, Irina Spiry, Benjamin Rue Wood, Dan Hancu, Wei ChenAbstract:GE Global Research is developing technology to remove carbon dioxide (CO 2) from the flue gas of coal-fired powerplants. A mixture of 3-aminopropyl end-capped polydimethylsiloxane (GAP-1m) and triethylene glycol (TEG) is the preferred CO2-capture solvent. GE Global Research was contracted by the Department of Energy to test a pilot-scale continuous CO2 absorption/desorption system using a GAP-1m/TEG mixture as the solvent. As part of that effort, an Environmental, Health, and Safety (EH&S) assessment for a CO2-capture system for a 550 MW coal-fired powerplant was conducted. Five components of the solvent, CAS#2469-55-8 (GAP-0), CAS#106214-84-0 (GAP-1-4), TEG, and methanol and xylene (minor contaminants from the aminosilicone) are included in this assessment. One by-product, GAP- 1m/SOX salt, and dodecylbenzenesulfonicacid (DDBSA) were also identified foranalysis. An EH&S assessment was also completed for the manufacturing process for the GAP-1m solvent. The chemicals associated with the manufacturing process include methanol, xylene, allyl chloride, potassium cyanate, sodium hydroxide (NaOH), tetramethyldisiloxane (TMDSO), tetramethyl ammonium hydroxide, Karstedt catalyst, octamethylcyclotetrasiloxane (D4), Aliquat 336, methyl carbamate, potassium chloride, trimethylamine, and (3-aminopropyl) dimethyl silanol. The toxicological effects of each component of both the CO2 capture system and the manufacturing process were defined, and control mechanisms necessary to comply with U.S. EH&S regulations aremore » summarized. Engineering and control systems, including environmental abatement, are described for minimizing exposure and release of the chemical components. Proper handling and storage recommendations are made for each chemical to minimize risk to workers and the surrounding community.« less
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a combined experimental and computational study on selected physical properties of Aminosilicones
Industrial & Engineering Chemistry Research, 2014Co-Authors: Robert James Perry, Irina Spiry, Sarah Elizabeth Genovese, Rachel L Farnum, Thomas M Perry, Michael Joseph Obrien, Deli Chen, Robert M Enick, Karl J Johnson, Saeed S AlshahraniAbstract:A number of physical properties of Aminosilicones have been determined experimentally and predicted computationally. It was found that COSMO-RS predicted the densities of the materials under study to within about 4% of the experimentally determined values. Vapor pressure measurements were performed, and all of the Aminosilicones of interest were found to be significantly less volatile than the benchmark MEA material. COSMO-RS was reasonably accurate for predicting the vapor pressures for Aminosilicones that were thermally stable. The heat capacities of all Aminosilicones tested were between 2.0 and 2.3 J/(g·°C); again substantially lower than a benchmark 30% aqueous MEA solution. Surface energies for the Aminosilicones were found to be 23.3–28.3 dyne/cm and were accurately predicted using the parachor method.
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Bench-Scale Silicone Process for Low-Cost CO{sub 2} Capture
2013Co-Authors: Ravi-kumar Vipperla, Ray Steele, Surinder Prabhjot Singh, Irina Spiry, Benjamin Rue WoodAbstract:A bench-scale system was designed and built to test an aminosilicone-based solvent. A model was built of the bench-scale system and this model was scaled up to model the performance of a carbon capture unit, using Aminosilicones, for CO{sub 2} capture and sequestration (CCS) for a pulverized coal (PC) boiler at 550 MW. System and economic analysis for the carbon capture unit demonstrates that the aminosilicone solvent has significant advantages relative to a monoethanol amine (MEA)-based system. The CCS energy penalty for MEA is 35.9% and the energy penalty for aminosilicone solvent is 30.4% using a steam temperature of 395 °C (743 °F). If the steam temperature is lowered to 204 °C (400 °F), the energy penalty for the aminosilicone solvent is reduced to 29%. The increase in cost of electricity (COE) over the non-capture case for MEA is ~109% and increase in COE for aminosilicone solvent is ~98 to 103% depending on the solvent cost at a steam temperature of 395 °C (743 °F). If the steam temperature is lowered to 204 °C (400 °F), the increase in COE for the aminosilicone solvent is reduced to ~95-100%.
Cláudio Augusto Oller Do Nascimento - One of the best experts on this subject based on the ideXlab platform.
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Degradation of an aminosilicone polymer in a water emulsion by the Fenton and the photochemically enhanced Fenton reactions
Chemical Engineering and Processing, 2005Co-Authors: Antonio Carlos S. C. Teixeira, Roberto Guardani, André M. Braun, Esther Oliveros, Cláudio Augusto Oller Do NascimentoAbstract:The degradation of a biologically persistent aminosilicone polymer (PDMAS) formulation, used in the textile industry as a softener of polyester fabrics, was investigated using the Fenton and the photochemically enhanced Fenton reactions. Experiments were performed using a commercially available aqueous silicone formulation (polymer-in-water emulsion stabilized by non-ionic surfactants). Emulsions containing a high PDMAS concentration (typical of textile processing) and a low PDMAS concentration (typical of end-processing wastewater) were investigated. In both cases, treatment by the Fenton and the photo-Fenton processes induced a phase separation after a relatively short reaction time, although the nature of the phase separation was different. Analyses of chemical oxygen demand (COD), nitrate, silicone and iron in the aqueous phase during treatment show that PDMAS (and/or partially oxidized PDMAS) was removed from the aqueous solution as a result of the phase separation process. Reaction pathways and mechanisms are discussed. Focusing on application, the occurrence of a phase separation may be advantageous for textile wastewater treatment, since this would enable the removal of PDMAS by conventional mechanical means.
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Photo‐Fenton Remediation of Wastewaters Containing Silicones: Experimental Study and Neural Network Modeling
Chemical Engineering & Technology, 2004Co-Authors: Antonio Carlos S. C. Teixeira, Roberto Guardani, Cláudio Augusto Oller Do NascimentoAbstract:The present work is aimed at the investigation of the photo-Fenton technology with regard to the remediation of diluted aqueous emulsions containing an aminosilicone polymer, in a bench-scale photochemical reactor. The experimental results show a strong interaction between temperature, light, Fe(II) and H 2 O 2 concentrations on the degradation process, which generates substances that might be readily biodegradable and/or a solid phase that is easily separated by simple mechanical operations. The neural network technique is an effective, simple approach to successfully modeling the photo-Fenton degradation system, in which thermal and photochemical reactions and related phenomena (such as solid precipitation) take place. The model might therefore be useful in process optimization, as well as in the design and scaleup of photochemical reactors for industrial application.
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solar photochemical degradation of Aminosilicones contained in liquid effluents process studies and neural network modeling
Industrial & Engineering Chemistry Research, 2003Co-Authors: Antonio Carlos S. C. Teixeira, And Roberto Guardani, Cláudio Augusto Oller Do NascimentoAbstract:The effectiveness of the solar-driven photo-Fenton process in treating wastewater contaminated with aminosilicone compounds has been evaluated in a parabolic trough reactor under variable weather conditions. On sunny days, after 3 h of irradiation, more than 80% of the initial COD has been removed. The degradation generates compounds that might be readily biodegradable and/or a solid phase that is easily separated by mechanical means. An important interaction between manipulated [H2O2 and Fe(II) concentrations] and nonmanipulated (direct and diffuse components of solar radiation) variables was detected. Therefore, degradation was possible even on cloudy days, provided that the H2O2 and Fe(II) concentrations are conveniently selected. The neural network technique is an effective, simple approach to successfully modeling the solar-driven photo-Fenton degradation. The model might therefore be useful in process optimization, as well as in the design and scale-up of solar reactors for industrial application.
Jason Louis Davis - One of the best experts on this subject based on the ideXlab platform.
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co2 capture using solutions of alkanolamines and Aminosilicones
Energy & Fuels, 2012Co-Authors: Robert James Perry, Jason Louis DavisAbstract:Tertiary amino alcohols have been shown to be effective co-solvents for CO2 capture when used in conjunction with Aminosilicones. In some cases, they demonstrated a marked increase in CO2 capture compared to an equivalent weight loading of triethylene glycol and also showed a lower viscosity at a given CO2 loading. These materials may be useful as co-solvents in carbon capture processes using Aminosilicones.
