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Drastic enhancement of carbon dioxide adsorption in fluoroalkyl-modified poly(allylamine)

Athanasios Koutsianos, Louise Hamdy, Chun-Jae Yoo, Jason J. Lee, Marco Taddei Orcid Logo, Jagoda M. Urban-Klaehn, Jerzy Dryzek, Christopher W. Jones Orcid Logo, Andrew Barron, Enrico Andreoli Orcid Logo

Journal of Materials Chemistry A, Volume: 9, Issue: 17, Pages: 10827 - 10837

Swansea University Authors: Athanasios Koutsianos, Louise Hamdy, Marco Taddei Orcid Logo, Andrew Barron, Enrico Andreoli Orcid Logo

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DOI (Published version): 10.1039/d1ta00879j

Abstract

Polyamine-based carbon dioxide sorbents suffer from a seesaw relationship between amine content and amine efficiency. High polyamine loadings equate to increased amine contents, but often at the expense of amine efficiency. Carbon dioxide mass transport in compact polymers is severely limited, espec...

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Published in: Journal of Materials Chemistry A
ISSN: 2050-7488 2050-7496
Published: Royal Society of Chemistry (RSC) 2021
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URI: https://cronfa.swan.ac.uk/Record/cronfa56797
first_indexed 2021-05-04T15:29:50Z
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High polyamine loadings equate to increased amine contents, but often at the expense of amine efficiency. Carbon dioxide mass transport in compact polymers is severely limited, especially at ambient temperature. High polymer contents curtail diffusion pathways, hindering CO2 from reaching and reacting with the numerous amine functions. Here, we overcome this issue using poly(allylamine) (PAA) grafted with short fluoroalkyl chains and then cross-linked with C60. As experimentally evidenced by positron annihilation lifetime spectroscopy, the incorporation of fluoroalkyl chains generates free volume elements that act as additional diffusion pathways within the material. The inclusion of void volume in fluoroalkyl-functionalized PAA sorbents results in radically increased CO2 uptakes and amine efficiencies in diluted gas streams at room temperature, including simulated air. We speculate that the hydrophobic fluorinated functions interfere with the strong amine hydrogen bonding network disrupting and consequently altering the packing and conformation of the polymer chains. The evidence presented here is a blueprint for the development of more efficient amine-based CO2 sorbents.</abstract><type>Journal Article</type><journal>Journal of Materials Chemistry A</journal><volume>9</volume><journalNumber>17</journalNumber><paginationStart>10827</paginationStart><paginationEnd>10837</paginationEnd><publisher>Royal Society of Chemistry (RSC)</publisher><placeOfPublication/><isbnPrint/><isbnElectronic/><issnPrint>2050-7488</issnPrint><issnElectronic>2050-7496</issnElectronic><keywords/><publishedDay>21</publishedDay><publishedMonth>4</publishedMonth><publishedYear>2021</publishedYear><publishedDate>2021-04-21</publishedDate><doi>10.1039/d1ta00879j</doi><url/><notes/><college>COLLEGE NANME</college><CollegeCode>COLLEGE CODE</CollegeCode><institution>Swansea University</institution><apcterm/><funders>Financial support was provided by the Reduce Industrial Carbon Emissions (RICE) and Flexible Integrated Energy Systems (FLEXIS) research operations part funded by the EU's European Regional Development Fund through the Welsh Government. We also acknowledge support from the SUSTAIN Manufacturing Hub funded by the Engineering and Physical Sciences Research Council (EP/S018107/1). Funding for the work of CJY, JJL and CWJ was provided in part by UNCAGE-ME, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under award no. DE-SC0012577. MT wish to acknowledge funding from the European Union's Horizon 2020 research and innovation programme under the Marie Sk&#x142;odowska-Curie grant agreement No 663830. 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spelling 2022-08-16T11:48:49.7701060 v2 56797 2021-05-04 Drastic enhancement of carbon dioxide adsorption in fluoroalkyl-modified poly(allylamine) 7d3db0003199a71fe03005e41899b42a Athanasios Koutsianos Athanasios Koutsianos true false 7f3a162e82c925cadead8a3b8d37dc81 Louise Hamdy Louise Hamdy true false 5cffd1038508554d8596dee8b4e51052 0000-0003-2805-6375 Marco Taddei Marco Taddei true false 92e452f20936d688d36f91c78574241d Andrew Barron Andrew Barron true false cbd843daab780bb55698a3daccd74df8 0000-0002-1207-2314 Enrico Andreoli Enrico Andreoli true false 2021-05-04 Polyamine-based carbon dioxide sorbents suffer from a seesaw relationship between amine content and amine efficiency. High polyamine loadings equate to increased amine contents, but often at the expense of amine efficiency. Carbon dioxide mass transport in compact polymers is severely limited, especially at ambient temperature. High polymer contents curtail diffusion pathways, hindering CO2 from reaching and reacting with the numerous amine functions. Here, we overcome this issue using poly(allylamine) (PAA) grafted with short fluoroalkyl chains and then cross-linked with C60. As experimentally evidenced by positron annihilation lifetime spectroscopy, the incorporation of fluoroalkyl chains generates free volume elements that act as additional diffusion pathways within the material. The inclusion of void volume in fluoroalkyl-functionalized PAA sorbents results in radically increased CO2 uptakes and amine efficiencies in diluted gas streams at room temperature, including simulated air. We speculate that the hydrophobic fluorinated functions interfere with the strong amine hydrogen bonding network disrupting and consequently altering the packing and conformation of the polymer chains. The evidence presented here is a blueprint for the development of more efficient amine-based CO2 sorbents. Journal Article Journal of Materials Chemistry A 9 17 10827 10837 Royal Society of Chemistry (RSC) 2050-7488 2050-7496 21 4 2021 2021-04-21 10.1039/d1ta00879j COLLEGE NANME COLLEGE CODE Swansea University Financial support was provided by the Reduce Industrial Carbon Emissions (RICE) and Flexible Integrated Energy Systems (FLEXIS) research operations part funded by the EU's European Regional Development Fund through the Welsh Government. We also acknowledge support from the SUSTAIN Manufacturing Hub funded by the Engineering and Physical Sciences Research Council (EP/S018107/1). Funding for the work of CJY, JJL and CWJ was provided in part by UNCAGE-ME, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under award no. DE-SC0012577. MT wish to acknowledge funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No 663830. JMU-K wish to acknowledge the project 18A12-210FP of the INL Laboratory Directed Research & Development (LDRD) program. 2022-08-16T11:48:49.7701060 2021-05-04T16:27:37.6748377 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemical Engineering Athanasios Koutsianos 1 Louise Hamdy 2 Chun-Jae Yoo 3 Jason J. Lee 4 Marco Taddei 0000-0003-2805-6375 5 Jagoda M. Urban-Klaehn 6 Jerzy Dryzek 7 Christopher W. Jones 0000-0003-3255-5791 8 Andrew Barron 9 Enrico Andreoli 0000-0002-1207-2314 10 56797__19797__83331c28a0fa48bc98f3a0aa77fe7638.pdf 56797.pdf 2021-05-04T16:29:21.0914491 Output 1167303 application/pdf Accepted Manuscript true 2022-04-21T00:00:00.0000000 true eng http://creativecommons.org/licenses/by-nc-nd/4.0/
title Drastic enhancement of carbon dioxide adsorption in fluoroalkyl-modified poly(allylamine)
spellingShingle Drastic enhancement of carbon dioxide adsorption in fluoroalkyl-modified poly(allylamine)
Athanasios Koutsianos
Louise Hamdy
Marco Taddei
Andrew Barron
Enrico Andreoli
title_short Drastic enhancement of carbon dioxide adsorption in fluoroalkyl-modified poly(allylamine)
title_full Drastic enhancement of carbon dioxide adsorption in fluoroalkyl-modified poly(allylamine)
title_fullStr Drastic enhancement of carbon dioxide adsorption in fluoroalkyl-modified poly(allylamine)
title_full_unstemmed Drastic enhancement of carbon dioxide adsorption in fluoroalkyl-modified poly(allylamine)
title_sort Drastic enhancement of carbon dioxide adsorption in fluoroalkyl-modified poly(allylamine)
author_id_str_mv 7d3db0003199a71fe03005e41899b42a
7f3a162e82c925cadead8a3b8d37dc81
5cffd1038508554d8596dee8b4e51052
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cbd843daab780bb55698a3daccd74df8
author_id_fullname_str_mv 7d3db0003199a71fe03005e41899b42a_***_Athanasios Koutsianos
7f3a162e82c925cadead8a3b8d37dc81_***_Louise Hamdy
5cffd1038508554d8596dee8b4e51052_***_Marco Taddei
92e452f20936d688d36f91c78574241d_***_Andrew Barron
cbd843daab780bb55698a3daccd74df8_***_Enrico Andreoli
author Athanasios Koutsianos
Louise Hamdy
Marco Taddei
Andrew Barron
Enrico Andreoli
author2 Athanasios Koutsianos
Louise Hamdy
Chun-Jae Yoo
Jason J. Lee
Marco Taddei
Jagoda M. Urban-Klaehn
Jerzy Dryzek
Christopher W. Jones
Andrew Barron
Enrico Andreoli
format Journal article
container_title Journal of Materials Chemistry A
container_volume 9
container_issue 17
container_start_page 10827
publishDate 2021
institution Swansea University
issn 2050-7488
2050-7496
doi_str_mv 10.1039/d1ta00879j
publisher Royal Society of Chemistry (RSC)
college_str Faculty of Science and Engineering
hierarchytype
hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Chemical Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemical Engineering
document_store_str 1
active_str 0
description Polyamine-based carbon dioxide sorbents suffer from a seesaw relationship between amine content and amine efficiency. High polyamine loadings equate to increased amine contents, but often at the expense of amine efficiency. Carbon dioxide mass transport in compact polymers is severely limited, especially at ambient temperature. High polymer contents curtail diffusion pathways, hindering CO2 from reaching and reacting with the numerous amine functions. Here, we overcome this issue using poly(allylamine) (PAA) grafted with short fluoroalkyl chains and then cross-linked with C60. As experimentally evidenced by positron annihilation lifetime spectroscopy, the incorporation of fluoroalkyl chains generates free volume elements that act as additional diffusion pathways within the material. The inclusion of void volume in fluoroalkyl-functionalized PAA sorbents results in radically increased CO2 uptakes and amine efficiencies in diluted gas streams at room temperature, including simulated air. We speculate that the hydrophobic fluorinated functions interfere with the strong amine hydrogen bonding network disrupting and consequently altering the packing and conformation of the polymer chains. The evidence presented here is a blueprint for the development of more efficient amine-based CO2 sorbents.
published_date 2021-04-21T14:02:37Z
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score 11.048149

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