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Adjustable Functionalization of Hyper-Cross-Linked Polymers of Intrinsic Microporosity for Enhanced CO2 Adsorption and Selectivity over N2 and CH4

Haoli Zhou, Christopher Rayer, Ariana Antonangelo, Tash Hawkins, Mariolino Carta Orcid Logo

ACS Applied Materials & Interfaces, Volume: 14, Issue: 18, Pages: 20997 - 21006

Swansea University Authors: Haoli Zhou, Ariana Antonangelo, Tash Hawkins, Mariolino Carta Orcid Logo

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DOI (Published version): 10.1021/acsami.2c02604

Abstract

In this paper, we report the design, synthesis, and characterization of a series of hyper-cross-linked polymers of intrinsic microporosity (PIMs), with high CO2 uptake and good CO2/N2 and CO2/CH4 selectivity, which makes them competitive for carbon capture and biogas upgrading. The starting hydrocar...

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Published in: ACS Applied Materials & Interfaces
ISSN: 1944-8244 1944-8252
Published: American Chemical Society (ACS) 2022
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URI: https://cronfa.swan.ac.uk/Record/cronfa59899
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The starting hydrocarbon polymers&#x2019; backbones were functionalized with groups such as &#x2212;NO2, &#x2212;NH2, and &#x2212;HSO3, with the aim of tuning their adsorption selectivity toward CO2 over nitrogen and methane. This led to a significant improvement in the performance in the potential separation of these gases. All polymers were characterized via Fourier transform infrared (FTIR) spectroscopy and 13C solid-state NMR to confirm their molecular structures and isothermal gas adsorption to assess their porosity, pore size distribution, and selectivity. The insertion of the functional groups resulted in an overall decrease in the porosity of the starting polymers, which was compensated with an improvement in the final CO2 uptake and selectivity over the chosen gases. The best uptakes were achieved with the sulfonated polymers, which reached up to 298 mg g&#x2013;1 (6.77 mmol g&#x2013;1), whereas the best CO2/N2 selectivities were recorded by the aminated polymers, which reached 26.5. Regarding CH4, the most interesting selectivities over CO2 were also obtained with the aminated PIMs, with values up to 8.6. The reason for the improvements was ascribed to a synergetic contribution of porosity, choice of the functional group, and optimal isosteric heat of adsorption of the materials.</abstract><type>Journal Article</type><journal>ACS Applied Materials &amp;amp; Interfaces</journal><volume>14</volume><journalNumber>18</journalNumber><paginationStart>20997</paginationStart><paginationEnd>21006</paginationEnd><publisher>American Chemical Society (ACS)</publisher><placeOfPublication/><isbnPrint/><isbnElectronic/><issnPrint>1944-8244</issnPrint><issnElectronic>1944-8252</issnElectronic><keywords>polymers of intrinsic microporosity, isothermal gas adsorption, pore size distribution, selectivity, isosteric heat</keywords><publishedDay>11</publishedDay><publishedMonth>5</publishedMonth><publishedYear>2022</publishedYear><publishedDate>2022-05-11</publishedDate><doi>10.1021/acsami.2c02604</doi><url/><notes/><college>COLLEGE NANME</college><department>Science and Engineering - Faculty</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>FGSEN</DepartmentCode><institution>Swansea University</institution><apcterm>SU Library paid the OA fee (TA Institutional Deal)</apcterm><funders>Swansea University Engineering and Physical Sciences Research Council - EP/T007362/1; China Scholarship Council - 201908320208</funders><projectreference/><lastEdited>2022-09-02T11:54:09.3297522</lastEdited><Created>2022-04-25T11:06:54.6183225</Created><path><level id="1">Faculty of Science and Engineering</level><level id="2">School of Engineering and Applied Sciences - Chemistry</level></path><authors><author><firstname>Haoli</firstname><surname>Zhou</surname><order>1</order></author><author><firstname>Christopher</firstname><surname>Rayer</surname><order>2</order></author><author><firstname>Ariana</firstname><surname>Antonangelo</surname><order>3</order></author><author><firstname>Tash</firstname><surname>Hawkins</surname><order>4</order></author><author><firstname>Mariolino</firstname><surname>Carta</surname><orcid>0000-0003-0718-6971</orcid><order>5</order></author></authors><documents><document><filename>59899__23918__744e386cdf02478086c897ca43d1f889.pdf</filename><originalFilename>59899.pdf</originalFilename><uploaded>2022-04-27T10:17:31.9813160</uploaded><type>Output</type><contentLength>3826166</contentLength><contentType>application/pdf</contentType><version>Version of Record</version><cronfaStatus>true</cronfaStatus><documentNotes>Released under the terms of a Creative Commons Attribution 4.0 International License (CC-BY 4.0).</documentNotes><copyrightCorrect>true</copyrightCorrect><language>eng</language><licence>https://creativecommons.org/licenses/by/4.0/</licence></document></documents><OutputDurs/></rfc1807>
spelling 2022-09-02T11:54:09.3297522 v2 59899 2022-04-25 Adjustable Functionalization of Hyper-Cross-Linked Polymers of Intrinsic Microporosity for Enhanced CO2 Adsorption and Selectivity over N2 and CH4 82af13a796d36cb6adf0e108c5c93648 Haoli Zhou Haoli Zhou true false 4565af0854d884b5f995af8f5dc652fc Ariana Antonangelo Ariana Antonangelo true false 504b1b0b26830fee1373ecc50801f01a Tash Hawkins Tash Hawkins true false 56aebf2bba457f395149bbecbfa6d3eb 0000-0003-0718-6971 Mariolino Carta Mariolino Carta true false 2022-04-25 FGSEN In this paper, we report the design, synthesis, and characterization of a series of hyper-cross-linked polymers of intrinsic microporosity (PIMs), with high CO2 uptake and good CO2/N2 and CO2/CH4 selectivity, which makes them competitive for carbon capture and biogas upgrading. The starting hydrocarbon polymers’ backbones were functionalized with groups such as −NO2, −NH2, and −HSO3, with the aim of tuning their adsorption selectivity toward CO2 over nitrogen and methane. This led to a significant improvement in the performance in the potential separation of these gases. All polymers were characterized via Fourier transform infrared (FTIR) spectroscopy and 13C solid-state NMR to confirm their molecular structures and isothermal gas adsorption to assess their porosity, pore size distribution, and selectivity. The insertion of the functional groups resulted in an overall decrease in the porosity of the starting polymers, which was compensated with an improvement in the final CO2 uptake and selectivity over the chosen gases. The best uptakes were achieved with the sulfonated polymers, which reached up to 298 mg g–1 (6.77 mmol g–1), whereas the best CO2/N2 selectivities were recorded by the aminated polymers, which reached 26.5. Regarding CH4, the most interesting selectivities over CO2 were also obtained with the aminated PIMs, with values up to 8.6. The reason for the improvements was ascribed to a synergetic contribution of porosity, choice of the functional group, and optimal isosteric heat of adsorption of the materials. Journal Article ACS Applied Materials &amp; Interfaces 14 18 20997 21006 American Chemical Society (ACS) 1944-8244 1944-8252 polymers of intrinsic microporosity, isothermal gas adsorption, pore size distribution, selectivity, isosteric heat 11 5 2022 2022-05-11 10.1021/acsami.2c02604 COLLEGE NANME Science and Engineering - Faculty COLLEGE CODE FGSEN Swansea University SU Library paid the OA fee (TA Institutional Deal) Swansea University Engineering and Physical Sciences Research Council - EP/T007362/1; China Scholarship Council - 201908320208 2022-09-02T11:54:09.3297522 2022-04-25T11:06:54.6183225 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry Haoli Zhou 1 Christopher Rayer 2 Ariana Antonangelo 3 Tash Hawkins 4 Mariolino Carta 0000-0003-0718-6971 5 59899__23918__744e386cdf02478086c897ca43d1f889.pdf 59899.pdf 2022-04-27T10:17:31.9813160 Output 3826166 application/pdf Version of Record true Released under the terms of a Creative Commons Attribution 4.0 International License (CC-BY 4.0). true eng https://creativecommons.org/licenses/by/4.0/
title Adjustable Functionalization of Hyper-Cross-Linked Polymers of Intrinsic Microporosity for Enhanced CO2 Adsorption and Selectivity over N2 and CH4
spellingShingle Adjustable Functionalization of Hyper-Cross-Linked Polymers of Intrinsic Microporosity for Enhanced CO2 Adsorption and Selectivity over N2 and CH4
Haoli Zhou
Ariana Antonangelo
Tash Hawkins
Mariolino Carta
title_short Adjustable Functionalization of Hyper-Cross-Linked Polymers of Intrinsic Microporosity for Enhanced CO2 Adsorption and Selectivity over N2 and CH4
title_full Adjustable Functionalization of Hyper-Cross-Linked Polymers of Intrinsic Microporosity for Enhanced CO2 Adsorption and Selectivity over N2 and CH4
title_fullStr Adjustable Functionalization of Hyper-Cross-Linked Polymers of Intrinsic Microporosity for Enhanced CO2 Adsorption and Selectivity over N2 and CH4
title_full_unstemmed Adjustable Functionalization of Hyper-Cross-Linked Polymers of Intrinsic Microporosity for Enhanced CO2 Adsorption and Selectivity over N2 and CH4
title_sort Adjustable Functionalization of Hyper-Cross-Linked Polymers of Intrinsic Microporosity for Enhanced CO2 Adsorption and Selectivity over N2 and CH4
author_id_str_mv 82af13a796d36cb6adf0e108c5c93648
4565af0854d884b5f995af8f5dc652fc
504b1b0b26830fee1373ecc50801f01a
56aebf2bba457f395149bbecbfa6d3eb
author_id_fullname_str_mv 82af13a796d36cb6adf0e108c5c93648_***_Haoli Zhou
4565af0854d884b5f995af8f5dc652fc_***_Ariana Antonangelo
504b1b0b26830fee1373ecc50801f01a_***_Tash Hawkins
56aebf2bba457f395149bbecbfa6d3eb_***_Mariolino Carta
author Haoli Zhou
Ariana Antonangelo
Tash Hawkins
Mariolino Carta
author2 Haoli Zhou
Christopher Rayer
Ariana Antonangelo
Tash Hawkins
Mariolino Carta
format Journal article
container_title ACS Applied Materials &amp; Interfaces
container_volume 14
container_issue 18
container_start_page 20997
publishDate 2022
institution Swansea University
issn 1944-8244
1944-8252
doi_str_mv 10.1021/acsami.2c02604
publisher American Chemical Society (ACS)
college_str Faculty of Science and Engineering
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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 - Chemistry{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemistry
document_store_str 1
active_str 0
description In this paper, we report the design, synthesis, and characterization of a series of hyper-cross-linked polymers of intrinsic microporosity (PIMs), with high CO2 uptake and good CO2/N2 and CO2/CH4 selectivity, which makes them competitive for carbon capture and biogas upgrading. The starting hydrocarbon polymers’ backbones were functionalized with groups such as −NO2, −NH2, and −HSO3, with the aim of tuning their adsorption selectivity toward CO2 over nitrogen and methane. This led to a significant improvement in the performance in the potential separation of these gases. All polymers were characterized via Fourier transform infrared (FTIR) spectroscopy and 13C solid-state NMR to confirm their molecular structures and isothermal gas adsorption to assess their porosity, pore size distribution, and selectivity. The insertion of the functional groups resulted in an overall decrease in the porosity of the starting polymers, which was compensated with an improvement in the final CO2 uptake and selectivity over the chosen gases. The best uptakes were achieved with the sulfonated polymers, which reached up to 298 mg g–1 (6.77 mmol g–1), whereas the best CO2/N2 selectivities were recorded by the aminated polymers, which reached 26.5. Regarding CH4, the most interesting selectivities over CO2 were also obtained with the aminated PIMs, with values up to 8.6. The reason for the improvements was ascribed to a synergetic contribution of porosity, choice of the functional group, and optimal isosteric heat of adsorption of the materials.
published_date 2022-05-11T04:17:33Z
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