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Laboratory Aging of a Dual Function Material (DFM) for Reactive CO2 Capture: Integrated Direct Air Capture (DAC) Under Various Ambient Conditions and In Situ Catalytic Conversion to Renewable Methane.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Laboratory Aging of a Dual Function Material (DFM) for Reactive CO2 Capture: Integrated Direct Air Capture (DAC) Under Various Ambient Conditions and In Situ Catalytic Conversion to Renewable Methane./
Author:	Abdallah, Monica.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2024,
Description:	100 p.
Notes:	Source: Dissertations Abstracts International, Volume: 85-06, Section: B.
Contained By:	Dissertations Abstracts International85-06B.
Subject:	Environmental engineering. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=30691763
ISBN:	9798381174830

Laboratory Aging of a Dual Function Material (DFM) for Reactive CO2 Capture: Integrated Direct Air Capture (DAC) Under Various Ambient Conditions and In Situ Catalytic Conversion to Renewable Methane.
Abdallah, Monica.

Laboratory Aging of a Dual Function Material (DFM) for Reactive CO2 Capture: Integrated Direct Air Capture (DAC) Under Various Ambient Conditions and In Situ Catalytic Conversion to Renewable Methane. - Ann Arbor : ProQuest Dissertations & Theses, 2024 - 100 p.

Source: Dissertations Abstracts International, Volume: 85-06, Section: B.

Thesis (Ph.D.)--Columbia University, 2024.

This item must not be sold to any third party vendors.

The response to climate change must include decisive and collaborative solutions that minimize global CO2 emissions and enable a shift to low-carbon energy (renewable electricity) and CO2-derived chemicals and fuels. A major challenge of minimizing fossil fuel use is producing critical chemicals and fuels for heavy industry and transportation in novel ways. These traditionally fossil-derived products can be derived from CO2 that is captured from point sources or the atmosphere. Reactive CO2 capture is an emerging area of research that focuses on developing materials and processes for CO2 capture and in situ conversion to valuable chemicals or fuels. By combining these two steps, costly and energy-intensive steps of conventional integrated capture and conversion schemes are eliminated, including sorbent regeneration, CO2 purification, pressurization, and transportation. These operations typically drive up the cost of capture and conversion processes, making them less economically attractive.The dual function material (DFM) is an Al2O3-supported, nano-dispersed catalyst and sorbent combination that demonstrates both capture and catalytic conversion properties, making reactive capture possible. Feasibility of the 1% Ru, 10% "Na2O"/Al2O3 DFM for CO2 direct air capture (DAC) and in situ catalytic methanation (DACM) has been demonstrated in previous work. Recent work has prioritized advanced laboratory testing and laboratory aging of this DFM under a variety of simulated ambient capture climates to assess the advantages and limitations of the material. A monolith was used as a structured support for the DFM to minimize reactor pressure drop, a particularly relevant challenge for DAC applications where large volumes of air must be processed to separate the small volume of CO2 (~ 400 ppm). Findings from DFM monolith studies (1% Ru, 10% "Na2O"/Al2O3//monolith) were shared with an engineering partner to support scale up efforts.Laboratory-simulated DACM cycles consisted of DAC performed at various real-world simulated ambient conditions followed by catalytic methanation, where the DFM was heated to 300°C in 15% H2/N2. Simulated DAC included O2 and humidity, and a surprising finding showed significant enhancement of CO2 adsorption due to humidity in the capture feed. The maximum CO2 capture capacity of the DFM monolith was measured to be 4.4 wt% (based on the weight of DFM material) at 25°C with 2 mol% H2O in the DAC feed. Aging studies revealed consistent CO2 capture and CH4 production after over 450 hours of cyclic DACM testing that included simulated ambient conditions. No signs of deactivation of either the "Na2O" sorbent or Ru catalyst were observed. The light-off temperature (indicative of kinetic control) observed for catalytic methanation was constant between fresh and aged cycles. These findings verified the qualifications of the 1% Ru, 10% "Na2O"/Al2O3//monolith for the DACM application and supported further advanced bench and pilot plant testing by our engineering collaborator.Additional parametric studies were conducted to evaluate the effects of varying humidity during DAC and revealed that a higher H2O concentration in the DAC feed correlates with greater CO2 captured and converted with no evidence of competitive adsorption between CO2 and H2O. Additionally, it was found that temperature changes within ambient range (0 - 40°C) played little role in varying CO2 captured under dry conditions, whereas moisture was found to be a major driver of capture capacity. Furthermore, stable performance at a reference condition was always achieved after excursions to varying ambient conditions.DACM tests revealed 30 - 40% of captured CO2 desorbs during the temperature swing step, which was attributed mainly to the slow heating rate and low H2 content (15%) required for safe laboratory operation. Unreacted CO2 was eliminated by shortening the DAC step and engaging partial capture capacity of the DFM. This mode of cycling is more representative of that which would be carried out at scale, as shorter adsorption durations capitalize on the fastest adsorption kinetics exhibited by a capture material. Consistent with reported literature, findings suggest that CO2 is preferentially adsorbed to stronger capture sites at the onset of DAC that are better able to retain CO2 during heat up. Though the DFM is not fully utilized, these partial capacity cycles demonstrated higher conversions to CH4 and a more efficient use of the material that will require less downstream purification at scale.

ISBN: 9798381174830Subjects--Topical Terms:

548583
Environmental engineering.
Subjects--Index Terms:

Catalysis

Laboratory Aging of a Dual Function Material (DFM) for Reactive CO2 Capture: Integrated Direct Air Capture (DAC) Under Various Ambient Conditions and In Situ Catalytic Conversion to Renewable Methane.
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520 $a The response to climate change must include decisive and collaborative solutions that minimize global CO2 emissions and enable a shift to low-carbon energy (renewable electricity) and CO2-derived chemicals and fuels. A major challenge of minimizing fossil fuel use is producing critical chemicals and fuels for heavy industry and transportation in novel ways. These traditionally fossil-derived products can be derived from CO2 that is captured from point sources or the atmosphere. Reactive CO2 capture is an emerging area of research that focuses on developing materials and processes for CO2 capture and in situ conversion to valuable chemicals or fuels. By combining these two steps, costly and energy-intensive steps of conventional integrated capture and conversion schemes are eliminated, including sorbent regeneration, CO2 purification, pressurization, and transportation. These operations typically drive up the cost of capture and conversion processes, making them less economically attractive.The dual function material (DFM) is an Al2O3-supported, nano-dispersed catalyst and sorbent combination that demonstrates both capture and catalytic conversion properties, making reactive capture possible. Feasibility of the 1% Ru, 10% "Na2O"/Al2O3 DFM for CO2 direct air capture (DAC) and in situ catalytic methanation (DACM) has been demonstrated in previous work. Recent work has prioritized advanced laboratory testing and laboratory aging of this DFM under a variety of simulated ambient capture climates to assess the advantages and limitations of the material. A monolith was used as a structured support for the DFM to minimize reactor pressure drop, a particularly relevant challenge for DAC applications where large volumes of air must be processed to separate the small volume of CO2 (~ 400 ppm). Findings from DFM monolith studies (1% Ru, 10% "Na2O"/Al2O3//monolith) were shared with an engineering partner to support scale up efforts.Laboratory-simulated DACM cycles consisted of DAC performed at various real-world simulated ambient conditions followed by catalytic methanation, where the DFM was heated to 300°C in 15% H2/N2. Simulated DAC included O2 and humidity, and a surprising finding showed significant enhancement of CO2 adsorption due to humidity in the capture feed. The maximum CO2 capture capacity of the DFM monolith was measured to be 4.4 wt% (based on the weight of DFM material) at 25°C with 2 mol% H2O in the DAC feed. Aging studies revealed consistent CO2 capture and CH4 production after over 450 hours of cyclic DACM testing that included simulated ambient conditions. No signs of deactivation of either the "Na2O" sorbent or Ru catalyst were observed. The light-off temperature (indicative of kinetic control) observed for catalytic methanation was constant between fresh and aged cycles. These findings verified the qualifications of the 1% Ru, 10% "Na2O"/Al2O3//monolith for the DACM application and supported further advanced bench and pilot plant testing by our engineering collaborator.Additional parametric studies were conducted to evaluate the effects of varying humidity during DAC and revealed that a higher H2O concentration in the DAC feed correlates with greater CO2 captured and converted with no evidence of competitive adsorption between CO2 and H2O. Additionally, it was found that temperature changes within ambient range (0 - 40°C) played little role in varying CO2 captured under dry conditions, whereas moisture was found to be a major driver of capture capacity. Furthermore, stable performance at a reference condition was always achieved after excursions to varying ambient conditions.DACM tests revealed 30 - 40% of captured CO2 desorbs during the temperature swing step, which was attributed mainly to the slow heating rate and low H2 content (15%) required for safe laboratory operation. Unreacted CO2 was eliminated by shortening the DAC step and engaging partial capture capacity of the DFM. This mode of cycling is more representative of that which would be carried out at scale, as shorter adsorption durations capitalize on the fastest adsorption kinetics exhibited by a capture material. Consistent with reported literature, findings suggest that CO2 is preferentially adsorbed to stronger capture sites at the onset of DAC that are better able to retain CO2 during heat up. Though the DFM is not fully utilized, these partial capacity cycles demonstrated higher conversions to CH4 and a more efficient use of the material that will require less downstream purification at scale.
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