Overcoming mass transfer limitations in cross-linked polyethyleneimine-based adsorbents to enable selective CO<sub>2</sub> capture at ambient temperature

Hamdy, Louise; GOUGSA, ABEL; Chow, Wing Ying; Russell, James; García-Díez, Enrique; Kulakova, Viktoriia; Garcia, Susana; Barron, Andrew; Taddei, Marco; Andreoli, Enrico

doi:10.1039/d1ma01072g

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Overcoming mass transfer limitations in cross-linked polyethyleneimine-based adsorbents to enable selective CO<sub>2</sub> capture at ambient temperature

Louise Hamdy, ABEL GOUGSA, Wing Ying Chow

, James Russell, Enrique García-Díez, Viktoriia Kulakova, Susana Garcia, Andrew Barron

, Marco Taddei

, Enrico Andreoli

Materials Advances, Volume: 3, Issue: 7, Pages: 3174 - 3191

Swansea University Authors: Louise Hamdy, ABEL GOUGSA, James Russell, Andrew Barron , Marco Taddei , Enrico Andreoli

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DOI (Published version): 10.1039/d1ma01072g

Abstract

New self-supported polyamine CO2 adsorbents are prepared by cross-linking branched polyethyleneimine (PEI) with 2,4,6-tris-(4-bromomethyl-3-fluoro-phenyl)-1,3,5-triazine (4BMFPT). Controlling the degree of cross-linking to ensure abundant free amine functionalities while maintaining a structure cond...

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Published in:	Materials Advances
ISSN:	2633-5409
Published:	Royal Society of Chemistry (RSC) 2022
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URI:	https://cronfa.swan.ac.uk/Record/cronfa60514
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Controlling the degree of cross-linking to ensure abundant free amine functionalities while maintaining a structure conducive to efficient mass transfer is key to accessing high CO2 adsorption and fast kinetics at ambient temperature. The polyamine-based adsorbent, PEI-4BMFPT, 10 : 1 (R), is composed of spherical particles up to 3 μm in diameter and demonstrates fast CO2 uptake of 2.31 mmol g−1 under 1 atm, 90% CO2/Ar at 30 °C. Its CO2/N2 selectivity, predicted by the ideal adsorbed solution theory is 575, equalling that of highly selective metal–organic frameworks. Based on humidified thermogravimetric analysis, it was observed that the presence of water promotes CO2 uptake capacity of 10 : 1 (R) to 3.27 mmol g−1 and results in strong chemisorption; likely by formation of ammonium carbonate and bicarbonate species. It is observed that CO2 uptake enhancement is highly subject to relative humidity and CO2 partial pressure conditions. When adsorption conditions combined low temperatures with low partial pressure CO2, 10 : 1 (R) showed reduced uptake. Tested under breakthrough conditions representative of post-combustion conditions, at 75% RH and 40 °C, CO2 uptake was reduced by 83% of the dry adsorption capacity. This body of work further advances the development of support-free CO2 adsorbents for ambient temperature applications and highlights the drastic effect that relative humidity and CO2 partial pressure have on uptake behaviour.</abstract><type>Journal Article</type><journal>Materials Advances</journal><volume>3</volume><journalNumber>7</journalNumber><paginationStart>3174</paginationStart><paginationEnd>3191</paginationEnd><publisher>Royal Society of Chemistry (RSC)</publisher><placeOfPublication/><isbnPrint/><isbnElectronic/><issnPrint/><issnElectronic>2633-5409</issnElectronic><keywords/><publishedDay>16</publishedDay><publishedMonth>2</publishedMonth><publishedYear>2022</publishedYear><publishedDate>2022-02-16</publishedDate><doi>10.1039/d1ma01072g</doi><url/><notes/><college>COLLEGE NANME</college><department>Engineering</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>EEN</DepartmentCode><institution>Swansea University</institution><apcterm>SU Library paid the OA fee (TA Institutional Deal)</apcterm><funders>This work is part of the Flexible Integrated Energy Systems (FLEXIS) and Reducing Industrial Carbon Emissions (RICE) research operations funded by the Welsh European Funding Office (WEFO) through the Welsh Government. Support was provided by the Engineering and Physical Sciences Research Council through the SUSTAIN Manufacturing Hub EP/S018107/1. Financial support was also provided by the Sêr Cymru Chair Programme and the Robert A. Welch Foundation (C-0002). We also acknowledge funding from European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement no 663830. The authors would like to acknowledge Stephen Shearan for assistance with material synthesis and Dr Matthew J. McPherson for assistance in performing BET measurements. We would like to acknowledge the assistance provided by Swansea University College of Engineering AIM Facility, which was funded in part by the EPSRC (EP/M028267/1), the European Regional Development Fund through the Welsh Government (80708) and the Ser Solar project via the Welsh Government. We acknowledge postdoctoral fellowship funding from the German Academic Exchange Service (DAAD) and Leibniz Association for WYC. This work benefited from access to the FMP Berlin NMR facility. 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spelling	2022-11-02T13:57:30.3415198 v2 60514 2022-07-16 Overcoming mass transfer limitations in cross-linked polyethyleneimine-based adsorbents to enable selective CO<sub>2</sub> capture at ambient temperature 7f3a162e82c925cadead8a3b8d37dc81 Louise Hamdy Louise Hamdy true false 4fc9cf9855219008513cdf648d489d63 ABEL GOUGSA ABEL GOUGSA true false 4ad47527c475ae228d69747c0c21f148 James Russell James Russell true false 92e452f20936d688d36f91c78574241d 0000-0002-2018-8288 Andrew Barron Andrew Barron true false 5cffd1038508554d8596dee8b4e51052 0000-0003-2805-6375 Marco Taddei Marco Taddei true false cbd843daab780bb55698a3daccd74df8 0000-0002-1207-2314 Enrico Andreoli Enrico Andreoli true false 2022-07-16 EEN New self-supported polyamine CO2 adsorbents are prepared by cross-linking branched polyethyleneimine (PEI) with 2,4,6-tris-(4-bromomethyl-3-fluoro-phenyl)-1,3,5-triazine (4BMFPT). Controlling the degree of cross-linking to ensure abundant free amine functionalities while maintaining a structure conducive to efficient mass transfer is key to accessing high CO2 adsorption and fast kinetics at ambient temperature. The polyamine-based adsorbent, PEI-4BMFPT, 10 : 1 (R), is composed of spherical particles up to 3 μm in diameter and demonstrates fast CO2 uptake of 2.31 mmol g−1 under 1 atm, 90% CO2/Ar at 30 °C. Its CO2/N2 selectivity, predicted by the ideal adsorbed solution theory is 575, equalling that of highly selective metal–organic frameworks. Based on humidified thermogravimetric analysis, it was observed that the presence of water promotes CO2 uptake capacity of 10 : 1 (R) to 3.27 mmol g−1 and results in strong chemisorption; likely by formation of ammonium carbonate and bicarbonate species. It is observed that CO2 uptake enhancement is highly subject to relative humidity and CO2 partial pressure conditions. When adsorption conditions combined low temperatures with low partial pressure CO2, 10 : 1 (R) showed reduced uptake. Tested under breakthrough conditions representative of post-combustion conditions, at 75% RH and 40 °C, CO2 uptake was reduced by 83% of the dry adsorption capacity. This body of work further advances the development of support-free CO2 adsorbents for ambient temperature applications and highlights the drastic effect that relative humidity and CO2 partial pressure have on uptake behaviour. Journal Article Materials Advances 3 7 3174 3191 Royal Society of Chemistry (RSC) 2633-5409 16 2 2022 2022-02-16 10.1039/d1ma01072g COLLEGE NANME Engineering COLLEGE CODE EEN Swansea University SU Library paid the OA fee (TA Institutional Deal) This work is part of the Flexible Integrated Energy Systems (FLEXIS) and Reducing Industrial Carbon Emissions (RICE) research operations funded by the Welsh European Funding Office (WEFO) through the Welsh Government. Support was provided by the Engineering and Physical Sciences Research Council through the SUSTAIN Manufacturing Hub EP/S018107/1. Financial support was also provided by the Sêr Cymru Chair Programme and the Robert A. Welch Foundation (C-0002). We also acknowledge funding from European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement no 663830. The authors would like to acknowledge Stephen Shearan for assistance with material synthesis and Dr Matthew J. McPherson for assistance in performing BET measurements. We would like to acknowledge the assistance provided by Swansea University College of Engineering AIM Facility, which was funded in part by the EPSRC (EP/M028267/1), the European Regional Development Fund through the Welsh Government (80708) and the Ser Solar project via the Welsh Government. We acknowledge postdoctoral fellowship funding from the German Academic Exchange Service (DAAD) and Leibniz Association for WYC. This work benefited from access to the FMP Berlin NMR facility. This work was also supported in part by the PrISMa Project (299659), funded through the ACT Programme (Accelerating CCS Technologies, Horizon 2020 Project 294766). 2022-11-02T13:57:30.3415198 2022-07-16T11:00:02.9836798 Faculty of Science and Engineering School of Engineering and Applied Sciences - Uncategorised Louise Hamdy 1 ABEL GOUGSA 2 Wing Ying Chow 0000-0003-0719-5958 3 James Russell 4 Enrique García-Díez 5 Viktoriia Kulakova 6 Susana Garcia 7 Andrew Barron 0000-0002-2018-8288 8 Marco Taddei 0000-0003-2805-6375 9 Enrico Andreoli 0000-0002-1207-2314 10 60514__24644__5d66b6f03d6f4dd3985567c388515c6b.pdf 60514.pdf 2022-07-19T16:01:16.8798037 Output 5038222 application/pdf Version of Record true This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. true eng http://creativecommons.org/licenses/by/3.0/
title	Overcoming mass transfer limitations in cross-linked polyethyleneimine-based adsorbents to enable selective CO<sub>2</sub> capture at ambient temperature
spellingShingle	Overcoming mass transfer limitations in cross-linked polyethyleneimine-based adsorbents to enable selective CO<sub>2</sub> capture at ambient temperature Louise Hamdy ABEL GOUGSA James Russell Andrew Barron Marco Taddei Enrico Andreoli
title_short	Overcoming mass transfer limitations in cross-linked polyethyleneimine-based adsorbents to enable selective CO<sub>2</sub> capture at ambient temperature
title_full	Overcoming mass transfer limitations in cross-linked polyethyleneimine-based adsorbents to enable selective CO<sub>2</sub> capture at ambient temperature
title_fullStr	Overcoming mass transfer limitations in cross-linked polyethyleneimine-based adsorbents to enable selective CO<sub>2</sub> capture at ambient temperature
title_full_unstemmed	Overcoming mass transfer limitations in cross-linked polyethyleneimine-based adsorbents to enable selective CO<sub>2</sub> capture at ambient temperature
title_sort	Overcoming mass transfer limitations in cross-linked polyethyleneimine-based adsorbents to enable selective CO<sub>2</sub> capture at ambient temperature
author_id_str_mv	7f3a162e82c925cadead8a3b8d37dc81 4fc9cf9855219008513cdf648d489d63 4ad47527c475ae228d69747c0c21f148 92e452f20936d688d36f91c78574241d 5cffd1038508554d8596dee8b4e51052 cbd843daab780bb55698a3daccd74df8
author_id_fullname_str_mv	7f3a162e82c925cadead8a3b8d37dc81_*_Louise Hamdy 4fc9cf9855219008513cdf648d489d63__ABEL GOUGSA 4ad47527c475ae228d69747c0c21f148__James Russell 92e452f20936d688d36f91c78574241d__Andrew Barron 5cffd1038508554d8596dee8b4e51052__Marco Taddei cbd843daab780bb55698a3daccd74df8_*_Enrico Andreoli
author	Louise Hamdy ABEL GOUGSA James Russell Andrew Barron Marco Taddei Enrico Andreoli
author2	Louise Hamdy ABEL GOUGSA Wing Ying Chow James Russell Enrique García-Díez Viktoriia Kulakova Susana Garcia Andrew Barron Marco Taddei Enrico Andreoli
format	Journal article
container_title	Materials Advances
container_volume	3
container_issue	7
container_start_page	3174
publishDate	2022
institution	Swansea University
issn	2633-5409
doi_str_mv	10.1039/d1ma01072g
publisher	Royal Society of Chemistry (RSC)
college_str	Faculty of Science and Engineering
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hierarchy_top_title	Faculty of Science and Engineering
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hierarchy_parent_title	Faculty of Science and Engineering
department_str	School of Engineering and Applied Sciences - Uncategorised{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Uncategorised
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description	New self-supported polyamine CO2 adsorbents are prepared by cross-linking branched polyethyleneimine (PEI) with 2,4,6-tris-(4-bromomethyl-3-fluoro-phenyl)-1,3,5-triazine (4BMFPT). Controlling the degree of cross-linking to ensure abundant free amine functionalities while maintaining a structure conducive to efficient mass transfer is key to accessing high CO2 adsorption and fast kinetics at ambient temperature. The polyamine-based adsorbent, PEI-4BMFPT, 10 : 1 (R), is composed of spherical particles up to 3 μm in diameter and demonstrates fast CO2 uptake of 2.31 mmol g−1 under 1 atm, 90% CO2/Ar at 30 °C. Its CO2/N2 selectivity, predicted by the ideal adsorbed solution theory is 575, equalling that of highly selective metal–organic frameworks. Based on humidified thermogravimetric analysis, it was observed that the presence of water promotes CO2 uptake capacity of 10 : 1 (R) to 3.27 mmol g−1 and results in strong chemisorption; likely by formation of ammonium carbonate and bicarbonate species. It is observed that CO2 uptake enhancement is highly subject to relative humidity and CO2 partial pressure conditions. When adsorption conditions combined low temperatures with low partial pressure CO2, 10 : 1 (R) showed reduced uptake. Tested under breakthrough conditions representative of post-combustion conditions, at 75% RH and 40 °C, CO2 uptake was reduced by 83% of the dry adsorption capacity. This body of work further advances the development of support-free CO2 adsorbents for ambient temperature applications and highlights the drastic effect that relative humidity and CO2 partial pressure have on uptake behaviour.
published_date	2022-02-16T04:18:41Z
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score	11.037056

Overcoming mass transfer limitations in cross-linked polyethyleneimine-based adsorbents to enable selective CO<sub>2</sub> capture at ambient temperature

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