Polyethylenimine-functionalized SBA-15 mesoporous silica for CO2 direct air capture and conversion to methane in a coupled catalytic reactor

Technologies that capture and store or utilize CO2 have the potential to reduce the concentration of this gas in the atmosphere or provide carbon-neutral energy vectors. In this work, materials based on mesoporous silica SBA-15 functionalized with different polyethylenimine (PEI) loadings, i.e. 30,...

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Main Authors: Iñigo Lacarra-Etxarri, Unai De La Torre, José A. González-Marcos, Juan R. González-Velasco, Beñat Pereda-Ayo
Format: Article
Language:English
Published: Elsevier 2025-07-01
Series:Journal of CO2 Utilization
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Online Access:http://www.sciencedirect.com/science/article/pii/S2212982025001180
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author Iñigo Lacarra-Etxarri
Unai De La Torre
José A. González-Marcos
Juan R. González-Velasco
Beñat Pereda-Ayo
author_facet Iñigo Lacarra-Etxarri
Unai De La Torre
José A. González-Marcos
Juan R. González-Velasco
Beñat Pereda-Ayo
author_sort Iñigo Lacarra-Etxarri
collection DOAJ
description Technologies that capture and store or utilize CO2 have the potential to reduce the concentration of this gas in the atmosphere or provide carbon-neutral energy vectors. In this work, materials based on mesoporous silica SBA-15 functionalized with different polyethylenimine (PEI) loadings, i.e. 30, 40 and 50 wt% were synthesized. The 50 wt% PEI/SBA-15 sample exhibited the highest CO2 capture capacity of 6.0 g CO2/100 g when exposed to 400 ppm CO2. The sorption performance in a capture unit feeding 420 ppm of CO2 showed negligible influence of the inclusion of 21 % oxygen, whereas 64 % humidity enhanced by 17 % the CO2 sorption capacity with respect to a dry feeding at 20 °C. Desorption of H2O preceded CO2 during temperature swing at 80 °C, revealing a stronger interaction of CO2 with the sorbent. Finally, experiments were conducted by coupling the capture unit with a downstream catalytic reactor loaded with 10 % Ni/Al2O3 catalyst. A gas stream composed of 420 ppm CO2, 21 % O2 and 64 % humidity was admitted to the capture unit working at 20 °C. The CO2 captured under direct air capture (DAC) conditions was desorbed in a 1 % H2/N2 gas stream by temperature swing at 80 °C. The desorption of H2O along with CO2 impeded the conversion of CO2 into CH4 in the reaction unit. The inclusion of an isothermal step at 45 °C during temperature swing allowed to decouple CO2 and H2O desorption, achieving a CO2 conversion of 80.4 % with a CH4 selectivity of 97.6 %.
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spelling doaj-art-1154fff2f6314dd6b5a344bf3d1b35f12025-08-20T03:26:39ZengElsevierJournal of CO2 Utilization2212-98392025-07-019710313410.1016/j.jcou.2025.103134Polyethylenimine-functionalized SBA-15 mesoporous silica for CO2 direct air capture and conversion to methane in a coupled catalytic reactorIñigo Lacarra-Etxarri0Unai De La Torre1José A. González-Marcos2Juan R. González-Velasco3Beñat Pereda-Ayo4Department of Chemical Engineering, Faculty of Science and Technology, Universidad del País Vasco UPV/EHU, Barrio Sarriena s/n, Leioa, Bizkaia 48940, SpainDepartment of Chemical Engineering, Faculty of Science and Technology, Universidad del País Vasco UPV/EHU, Barrio Sarriena s/n, Leioa, Bizkaia 48940, SpainDepartment of Chemical Engineering, Faculty of Science and Technology, Universidad del País Vasco UPV/EHU, Barrio Sarriena s/n, Leioa, Bizkaia 48940, SpainDepartment of Chemical Engineering, Faculty of Science and Technology, Universidad del País Vasco UPV/EHU, Barrio Sarriena s/n, Leioa, Bizkaia 48940, SpainCorresponding author.; Department of Chemical Engineering, Faculty of Science and Technology, Universidad del País Vasco UPV/EHU, Barrio Sarriena s/n, Leioa, Bizkaia 48940, SpainTechnologies that capture and store or utilize CO2 have the potential to reduce the concentration of this gas in the atmosphere or provide carbon-neutral energy vectors. In this work, materials based on mesoporous silica SBA-15 functionalized with different polyethylenimine (PEI) loadings, i.e. 30, 40 and 50 wt% were synthesized. The 50 wt% PEI/SBA-15 sample exhibited the highest CO2 capture capacity of 6.0 g CO2/100 g when exposed to 400 ppm CO2. The sorption performance in a capture unit feeding 420 ppm of CO2 showed negligible influence of the inclusion of 21 % oxygen, whereas 64 % humidity enhanced by 17 % the CO2 sorption capacity with respect to a dry feeding at 20 °C. Desorption of H2O preceded CO2 during temperature swing at 80 °C, revealing a stronger interaction of CO2 with the sorbent. Finally, experiments were conducted by coupling the capture unit with a downstream catalytic reactor loaded with 10 % Ni/Al2O3 catalyst. A gas stream composed of 420 ppm CO2, 21 % O2 and 64 % humidity was admitted to the capture unit working at 20 °C. The CO2 captured under direct air capture (DAC) conditions was desorbed in a 1 % H2/N2 gas stream by temperature swing at 80 °C. The desorption of H2O along with CO2 impeded the conversion of CO2 into CH4 in the reaction unit. The inclusion of an isothermal step at 45 °C during temperature swing allowed to decouple CO2 and H2O desorption, achieving a CO2 conversion of 80.4 % with a CH4 selectivity of 97.6 %.http://www.sciencedirect.com/science/article/pii/S2212982025001180Direct air capturePolyethylenimineSBA-15Carbon capture and utilizationCO2 sorption and conversion to CH4
spellingShingle Iñigo Lacarra-Etxarri
Unai De La Torre
José A. González-Marcos
Juan R. González-Velasco
Beñat Pereda-Ayo
Polyethylenimine-functionalized SBA-15 mesoporous silica for CO2 direct air capture and conversion to methane in a coupled catalytic reactor
Journal of CO2 Utilization
Direct air capture
Polyethylenimine
SBA-15
Carbon capture and utilization
CO2 sorption and conversion to CH4
title Polyethylenimine-functionalized SBA-15 mesoporous silica for CO2 direct air capture and conversion to methane in a coupled catalytic reactor
title_full Polyethylenimine-functionalized SBA-15 mesoporous silica for CO2 direct air capture and conversion to methane in a coupled catalytic reactor
title_fullStr Polyethylenimine-functionalized SBA-15 mesoporous silica for CO2 direct air capture and conversion to methane in a coupled catalytic reactor
title_full_unstemmed Polyethylenimine-functionalized SBA-15 mesoporous silica for CO2 direct air capture and conversion to methane in a coupled catalytic reactor
title_short Polyethylenimine-functionalized SBA-15 mesoporous silica for CO2 direct air capture and conversion to methane in a coupled catalytic reactor
title_sort polyethylenimine functionalized sba 15 mesoporous silica for co2 direct air capture and conversion to methane in a coupled catalytic reactor
topic Direct air capture
Polyethylenimine
SBA-15
Carbon capture and utilization
CO2 sorption and conversion to CH4
url http://www.sciencedirect.com/science/article/pii/S2212982025001180
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