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Developing Versatile Contactors for Direct Air Capture of CO(2) through Amine Grafting onto Alumina Pellets and Alumina Wash-Coated Monoliths

[Image: see text] The optimization of the air–solid contactor is critical to improve the efficiency of the direct air capture (DAC) process. To enable comparison of contactors and therefore a step toward optimization, two contactors are prepared in the form of pellets and wash-coated honeycomb monol...

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Autores principales: Grossmann, Quirin, Stampi-Bombelli, Valentina, Yakimov, Alexander, Docherty, Scott, Copéret, Christophe, Mazzotti, Marco
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10472440/
https://www.ncbi.nlm.nih.gov/pubmed/37663169
http://dx.doi.org/10.1021/acs.iecr.3c01265
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author Grossmann, Quirin
Stampi-Bombelli, Valentina
Yakimov, Alexander
Docherty, Scott
Copéret, Christophe
Mazzotti, Marco
author_facet Grossmann, Quirin
Stampi-Bombelli, Valentina
Yakimov, Alexander
Docherty, Scott
Copéret, Christophe
Mazzotti, Marco
author_sort Grossmann, Quirin
collection PubMed
description [Image: see text] The optimization of the air–solid contactor is critical to improve the efficiency of the direct air capture (DAC) process. To enable comparison of contactors and therefore a step toward optimization, two contactors are prepared in the form of pellets and wash-coated honeycomb monoliths. The desired amine functionalities are successfully incorporated onto these industrially relevant pellets by means of a procedure developed for powders, providing materials with a CO(2) uptake not influenced by the morphology and the structure of the materials according to the sorption measurements. Furthermore, the amine functionalities are incorporated onto alumina wash-coated monoliths that provide a similar CO(2) uptake compared to the pellets. Using breakthrough measurements, dry CO(2) uptakes of 0.44 and 0.4 mmol g(sorbent)(–1) are measured for pellets and for a monolith, respectively. NMR and IR studies of CO(2) uptake show that the CO(2) adsorbs mainly in the form of ammonium carbamate. Both contactors are characterized by estimated Toth isotherm parameters and linear driving force (LDF) coefficients to enable an initial comparison and provide information for further studies of the two contactors. LDF coefficients of 1.5 × 10(–4) and of 1.2 × 10(–3) s(–1) are estimated for the pellets and for a monolith, respectively. In comparison to the pellets, the monolith therefore exhibits particularly promising results in terms of adsorption kinetics due to its hierarchical pore structure. This is reflected in the productivity of the adsorption step of 6.48 mol m(–3) h(–1) for the pellets compared to 7.56 mol m(–3) h(–1) for the monolith at a pressure drop approximately 1 order of magnitude lower, making the monoliths prime candidates to enhance the efficiency of DAC processes.
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spelling pubmed-104724402023-09-02 Developing Versatile Contactors for Direct Air Capture of CO(2) through Amine Grafting onto Alumina Pellets and Alumina Wash-Coated Monoliths Grossmann, Quirin Stampi-Bombelli, Valentina Yakimov, Alexander Docherty, Scott Copéret, Christophe Mazzotti, Marco Ind Eng Chem Res [Image: see text] The optimization of the air–solid contactor is critical to improve the efficiency of the direct air capture (DAC) process. To enable comparison of contactors and therefore a step toward optimization, two contactors are prepared in the form of pellets and wash-coated honeycomb monoliths. The desired amine functionalities are successfully incorporated onto these industrially relevant pellets by means of a procedure developed for powders, providing materials with a CO(2) uptake not influenced by the morphology and the structure of the materials according to the sorption measurements. Furthermore, the amine functionalities are incorporated onto alumina wash-coated monoliths that provide a similar CO(2) uptake compared to the pellets. Using breakthrough measurements, dry CO(2) uptakes of 0.44 and 0.4 mmol g(sorbent)(–1) are measured for pellets and for a monolith, respectively. NMR and IR studies of CO(2) uptake show that the CO(2) adsorbs mainly in the form of ammonium carbamate. Both contactors are characterized by estimated Toth isotherm parameters and linear driving force (LDF) coefficients to enable an initial comparison and provide information for further studies of the two contactors. LDF coefficients of 1.5 × 10(–4) and of 1.2 × 10(–3) s(–1) are estimated for the pellets and for a monolith, respectively. In comparison to the pellets, the monolith therefore exhibits particularly promising results in terms of adsorption kinetics due to its hierarchical pore structure. This is reflected in the productivity of the adsorption step of 6.48 mol m(–3) h(–1) for the pellets compared to 7.56 mol m(–3) h(–1) for the monolith at a pressure drop approximately 1 order of magnitude lower, making the monoliths prime candidates to enhance the efficiency of DAC processes. American Chemical Society 2023-08-15 /pmc/articles/PMC10472440/ /pubmed/37663169 http://dx.doi.org/10.1021/acs.iecr.3c01265 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Grossmann, Quirin
Stampi-Bombelli, Valentina
Yakimov, Alexander
Docherty, Scott
Copéret, Christophe
Mazzotti, Marco
Developing Versatile Contactors for Direct Air Capture of CO(2) through Amine Grafting onto Alumina Pellets and Alumina Wash-Coated Monoliths
title Developing Versatile Contactors for Direct Air Capture of CO(2) through Amine Grafting onto Alumina Pellets and Alumina Wash-Coated Monoliths
title_full Developing Versatile Contactors for Direct Air Capture of CO(2) through Amine Grafting onto Alumina Pellets and Alumina Wash-Coated Monoliths
title_fullStr Developing Versatile Contactors for Direct Air Capture of CO(2) through Amine Grafting onto Alumina Pellets and Alumina Wash-Coated Monoliths
title_full_unstemmed Developing Versatile Contactors for Direct Air Capture of CO(2) through Amine Grafting onto Alumina Pellets and Alumina Wash-Coated Monoliths
title_short Developing Versatile Contactors for Direct Air Capture of CO(2) through Amine Grafting onto Alumina Pellets and Alumina Wash-Coated Monoliths
title_sort developing versatile contactors for direct air capture of co(2) through amine grafting onto alumina pellets and alumina wash-coated monoliths
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10472440/
https://www.ncbi.nlm.nih.gov/pubmed/37663169
http://dx.doi.org/10.1021/acs.iecr.3c01265
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