Development of amine-functionalized adsorbent for carbon dioxide capture from atmospheric air
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1 Research Collection Doctoral Thesis Development of amine-functionalized adsorbent for carbon dioxide capture from atmospheric air Author(s): Gebald, Christoph Publication Date: 2014 Permanent Link: Rights / License: In Copyright - Non-Commercial Use Permitted This page was generated automatically upon download from the ETH Zurich Research Collection. For more information please consult the Terms of use. ETH Library
2 Diss. ETH No DEVELOPMENT OF AMINE-FUNCTIONALIZED ADSORBENT FOR CARBON DIOXIDE CAPTURE FROM ATMOSPHERIC AIR A dissertation submitted to attain the degree of DOCTOR OF SCIENCES of ETH ZURICH (Dr. sc. ETH Zurich) presented by CHRISTOPH GEBALD MSc ETH ME, ETH Zurich born on April 03, 1983 citizen of Germany accepted on the recommendation of Prof. Dr. Aldo Steinfeld Dr. Tanja Zimmermann 2014
3 Abstract A novel amine-functionalized adsorbent for the direct capture of CO 2 from air (DAC) was developed, which uses biogenic raw materials and an environmentally benign synthesis route without organic solvents. The adsorbent was synthesized through freeze drying an aqueous suspension of nanofibrillated cellulose (NFC) and an aminosilane. A screening of commercial aminosilane moieties revealed that 3-aminopropylmethyldiethoxysilane (APDES) and N-(2-aminoethyl)-3- aminopropylmethyldimethoxysilane (AEAPDMS) are feasible to yield high capacity DAC adsorbents. At a CO 2 concentration of 506 ppm in air and a relative humidity of 40 % at 298 K, AEAPDMS-functionalized NFC adsorbed 1.39 mmol CO 2 /g after 12 h CO 2 adsorption in a packed bed arrangement. A fundamental analysis of single-component and binary CO 2 and H 2 O adsorption of amine-functionalized NFC was carried out in the temperature range K and at CO 2 partial pressures in the range kpa, where the ultralow partial pressure range is relevant for DAC. Single-component CO 2 and H 2 O adsorption experimental data were fitted to the Toth and Guggenheim- Anderson-de Boer models, respectively. Corresponding heats of adsorption, derived from explicit solutions of the van t Hoff equation, were -50 kj/mol CO 2 and -49 kj/mol H 2 O. Binary CO 2 /H 2 O adsorption measurements for humid air revealed that the presence of H 2 O at 2.55 kpa enhances CO 2 adsorption, while the presence of CO 2 at kpa does not influence H 2 O adsorption. Consequently H 2 O adsorption for DAC is solely driven by the relative humidity of the air during CO 2 adsorption. It was found that H 2 O adsorption increased significantly with increasing relative humidity of the air. Therefore the energy demand of the temperature-vacuum-swing (TVS) adsorption/desorption cycle for delivering pure CO 2 from air increases significantly with increasing relative humidity and urges the need to reduce the hygroscopy of the adsorbent. Finally, the chemical and physical stability of amine-functionalized NFC was investigated during TVS cycling. The presence of O 2 at 363 K degraded the adsorbent, reducing its CO 2 adsorption capacity by 30 % after 15 h of treatment in moist air with a dew point of 295 K. In contrast, exposure to moist CO 2 at 363 K with a dew point of 295 K did not deteriorate its CO 2 adsorption capacity after 15
4 ii Abstract h. Performing 100 TVS consecutive cycles, with CO 2 adsorption from ambient air containing ppm CO 2 at 303 K and 60 % relative humidity and with CO 2 desorption at 363 K and 30 mbar, resulted in a reduction of the equilibrium CO 2 adsorption capacity by maximum 5 %. The average CO 2 adsorption capacity during TVS cyclic operation was 0.90 mmol CO 2 /g.
5 Zusammenfassung Die vorliegende Arbeit stellt einen neuheitlichen aminfunktionalisierten Adsorbens vor, der für CO 2 Abscheidung aus der Atmosphäre (DAC) entwickelt wurde und der biogene Ausgangsmaterialien und ein umweltfreundliches Herstellverfahren ohne organische Lösungsmittel verwendet. Der Adsorbens wurde durch Gefriertrocknung einer Suspension bestehend aus nanofibrillierter Zellulose (NFC) und einem Aminosilan hergestellt. Eine Prüfung kommerzieller Aminosilane ergab, dass 3-aminopropylmethyldiethoxysilan (APDES) und N-(2- aminoethyl)-3-aminopropylmethyldimethoxysilan (AEAPDMS) besonders geeignet für die Herstellung eines DAC Adsorbens mit hoher CO 2 Kapazität sind. Bei einer CO 2 Konzentration von 506 ppm in Luft und einer relativen Luftfeuchtigkeit von 40 % bei einer Temperatur von 298 K, adsorbierte AEAPDMS-funktionalisierte NFC 1.39 mmol CO 2 /g nach 12 h CO 2 Adsorption in einem Schüttgutbett. Es wurde eine fundamentale Analyse von Einkomponenten und Zweikomponenten CO 2 und H 2 O Adsorption von aminfunktionalisierter NFC im Temperaturbereich K und im CO 2 Partialdruckbereich kpa durchgeführt, wobei der tiefe CO 2 Partialdruckbereich relevant für DAC ist. Experimentelle Messdaten der Einkomponenten CO 2 und H 2 O Adsorption wurden jeweils mit dem Toth und Guggenheim-Anderson-de Boer Modell modelliert. Die entsprechenden Adsorptionswärmen, welche als explizite Lösungen der van t Hoff Gleichung berechnet wurden, waren -50 kj/mol CO 2 und -49 kj/mol H 2 O. Zweikomponenten CO 2 /H 2 O Adsorption von feuchter Luft zeigte, dass Luftfeuchtigkeit mit einem Partialdruck von 2.55 kpa die CO 2 Adsorption verstärkte, wohingegen CO 2 mit einem Partialdruck von kpa keinen Einfluss auf die H 2 O Adsorption hatte. Damit ist die H 2 O Adsorption für DAC einzig von der relativen Luftfeuchtigkeit der Luft während der CO 2 Adsorption bestimmt. Es wurde festgestellt, dass die H 2 O Adsorption stark mit steigender relativer Luftfeuchtigkeit der Luft ansteigt. Daraus folgt, dass der Energieverbrauch von Adsorption/Desorption Zyklen basierend auf einem Temperatur-Vakuum- Wechselverfahren (TVS), welches während der Desorption hochreines CO 2 zur
6 iv Zusammenfassung Verfügung stellt, signifikant mit steigender relativer Luftfeuchtigkeit ansteigt und somit die Notwendigkeit von reduzierter Hygroskopie des Adsorbens aufzeigt. Schliesslich wurde die chemische und physikalische Stabilität von aminfunktionalisierter NFC während TVS Zyklen untersucht. Die Präsenz von O 2 bei einer Temperatur von 363 K degradiert den Adsorbens, so dass die CO 2 Kapazität nach 15 h Behandlung in feuchter Luft mit einem Taupunkt von 295 K um 30 % abgenommen hatte. Im Gegensatz dazu führte Kontakt mit feuchtem CO 2 mit einem Taupunkt von 295 K nach 15 h Behandlung bei 363 K zu keinem CO 2 Kapazitätsverlust. Nach 100 TVS Zyklen in Folge, wobei CO 2 Adsorption von Umgebungsluft mit einer CO 2 Konzentration von ppm bei 303 K und 60 % Luftfeuchtigkeit und CO 2 Desorption bei 363 K und 30 mbar durchgeführt wurden, war der Verlust der CO 2 Kapazität maximal 5 %. Die durchschnittliche CO 2 Adsorptionskapzität während der TVS Zyklen war 0.90 mmol CO 2 /g
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Research Collection Doctoral Thesis Design of adaptive structures with piezoelectric materials Author(s): Delpero, Tommaso Publication Date: 2014 Permanent Link: https://doi.org/10.3929/ethz-a-010183127
Grow rich and clean up later? Joint effects of international integration and democracy on environmental quality in developing countries
Research Collection Doctoral Thesis Grow rich and clean up later? Joint effects of international integration and democracy on environmental quality in developing countries Author(s): Ruoff, Gabriele Publication
Development of Models for Biomolecular Simulation: Polarisability and Solvation
Research Collection Doctoral Thesis Development of Models for Biomolecular Simulation: Polarisability and Solvation Author(s): Bachmann, Stephan Jan Publication Date: 2014 Permanent Link: https://doi.org/10.3929/ethz-a-010220737
Research Collection. The role of type I interferon signaling on T cells during acute viral infections. Doctoral Thesis.
Research Collection Doctoral Thesis The role of type I interferon signaling on T cells during acute viral infections Author(s): Crouse, Joshua Mark Publication Date: 2014 Permanent Link: https://doi.org/10.3929/ethz-a-010252591
Research Collection. Improving geometric calibration methods for multi-axis machining centers by examining error interdependencies effects
Research Collection Doctoral Thesis Improving geometric calibration methods for multi-axis machining centers by examining error interdependencies effects Author(s): Bringmann, Bernhard Publication Date:
Kinetic Framework of Spindle Assembly Checkpoint Signalling
Research Collection Doctoral Thesis Kinetic Framework of Spindle Assembly Checkpoint Signalling Author(s): Dick, Amalie Elisabeth Publication Date: 2014 Permanent Link: https://doi.org/10.3929/ethz-a-010198160
Sterilisation von stückigen Lebensmitteln mit Mikrowellen
Research Collection Doctoral Thesis Sterilisation von stückigen Lebensmitteln mit Mikrowellen Author(s): Spreng, Hans Publication Date: 1975 Permanent Link: https://doi.org/10.3929/ethza000119193 Rights
Shear band propagation in soils and dynamics of tsunamigenic landslides
Research Collection Doctoral Thesis Shear band propagation in soils and dynamics of tsunamigenic landslides Author(s): Saurer, Erich Publication Date: 2009 Permanent Link: https://doi.org/10.3929/ethz-a-005951122
Probing dark matter with strong gravitational lensing
Research Collection Doctoral Thesis Probing dark matter with strong gravitational lensing Author(s): Birrer, Simon Publication Date: 2016 Permanent Link: https://doi.org/10.3929/ethz-a-010861709 Rights
Radiation Grafted Fuel Cell Membranes with Improved Oxidative Stability
Diss. ETH No. 16995 Radiation Grafted Fuel Cell Membranes with Improved Oxidative Stability A dissertation submitted to the SWISS FEDERAL INSTITUTE OF TECHNOLOGY For the deg ree of DOCTOR OF SCIENCES presented
On document-centered mathematical component software
Research Collection Doctoral Thesis On document-centered mathematical component software Author(s): Weck, Wolfgang Publication Date: 1996 Permanent Link: https://doi.org/10.3929/ethz-a-001710334 Rights
Research Collection. Exploration of augmented reality technology for surgical training simulators. Doctoral Thesis. ETH Library
Research Collection Doctoral Thesis Exploration of augmented reality technology for surgical training simulators Author(s): Bianchi, Gérald Publication Date: 2007 Permanent Link: https://doi.org/10.3929/ethz-a-005307590
Ueber die Zusammensetzung, das Alterungsverhalten und die Inhibierung von Isolierölen
Research Collection Doctoral Thesis Ueber die Zusammensetzung, das Alterungsverhalten und die Inhibierung von Isolierölen Author(s): Künzli, Max Publication Date: 1967 Permanent Link: https://doi.org/10.3929/ethz-a-000087846
On the nature of pleiotropy and its role for adaptation
Research Collection Doctoral Thesis On the nature of pleiotropy and its role for adaptation Author(s): Polster, Robert Publication Date: 2013 Permanent Link: https://doi.org/10.3929/ethz-a-010006485 Rights
Research Collection. Doctoral Thesis. ETH Library. Author(s): Baettig, Julia. Publication Date: 2014
Research Collection Doctoral Thesis Sequential Coating of Nanopores with Charged Polymers: A General Approach for Controlling Pore Properties of Self- Assembled Block Copolymer Membranes Author(s): Baettig,
Research Collection. Doctoral Thesis. ETH Library. Author(s): Martens, Hans Jörg. Publication Date: 1978
Research Collection Doctoral Thesis Eine Verallgemeinerung des Begriffs der scheinbaren Aktivierungsenergie für Kriechen in halbempirischen Ansätzen und deren Anwendung auf das Kriechverhalten der grobzweiphasigen
The measurement of the oxygenation status of the newborn infant
Research Collection Doctoral Thesis The measurement of the oxygenation status of the newborn infant Author(s): Wolf, Martin Peter Publication Date: 1996 Permanent Link: https://doi.org/10.3929/ethz-a-001630372
Resource management in a multicore operating system
Research Collection Doctoral Thesis Resource management in a multicore operating system Author(s): Peter, Simon Publication Date: 2012 Permanent Link: https://doi.org/10.3929/ethz-a-007579246 Rights /
Location fingerprinting for ultra-wideband systems The key to efficient and robust localization
Research Collection Doctoral Thesis Location fingerprinting for ultra-wideband systems The key to efficient and robust localization Author(s): Steiner, Christoph Publication Date: 2010 Permanent Link:
Power Subsystem Design and Management for Solar Energy Harvesting Embedded Systems
Research Collection Doctoral Thesis Power Subsystem Design and Management for Solar Energy Harvesting Embedded Systems Author(s): Buchli, Bernhard R. Publication Date: 2015 Permanent Link: https://doi.org/10.3929/ethz-a-010476716
Research Collection. A novel biofuel cell harvesting electrical energy from activated human macrophages. Doctoral Thesis.
Research Collection Doctoral Thesis A novel biofuel cell harvesting electrical energy from activated human macrophages Author(s): Sakai Stalder, Miho Publication Date: 2009 Permanent Link: https://doi.org/10.3929/ethz-a-006020938
Characterization of the Endosomal Protein Vps13 as a suppressor of the ER-Mitochondria Encounter Structure
Research Collection Doctoral Thesis Characterization of the Endosomal Protein Vps13 as a suppressor of the ER-Mitochondria Encounter Structure Author(s): Lang, Alexander Publication Date: 2015 Permanent