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A new approach to enhancing the CO2 capture performance of defective UiO-66 via post-synthetic defect exchange

Athanasios Koutsianos, Ewa Kazimierska, Andrew Barron Orcid Logo, Marco Taddei Orcid Logo, Enrico Andreoli Orcid Logo

Dalton Transactions, Volume: 48, Issue: 10, Pages: 3349 - 3359

Swansea University Authors: Ewa Kazimierska, Andrew Barron Orcid Logo, Marco Taddei Orcid Logo, Enrico Andreoli Orcid Logo

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DOI (Published version): 10.1039/C9DT00154A

Abstract

Zirconium-based metal-organic frameworks (Zr-MOFs) are a subclass of MOFs known for their remarkable stability, especially in the presence of water. This makes them extremely attractive for practical applications, including CO2 capture from industrial emission sources; however, the CO2 adsorption ca...

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Published in: Dalton Transactions
ISSN: 1477-9226 1477-9234
Published: 2019
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URI: https://cronfa.swan.ac.uk/Record/cronfa48825
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This makes them extremely attractive for practical applications, including CO2 capture from industrial emission sources; however, the CO2 adsorption capacity of Zr-MOFs is moderate compared to that of the best performing MOFs reported to date. Functionalization of Zr-MOFs with amino groups has been demonstrated to increase their affinity for CO2. In this work, we assessed the potential of post-synthetic defect exchange (PSDE) as an alternative approach to introduce amino functionalities at missing-cluster defective sites in formic acid modulated UiO-66. Both pyridine-containing (picolinic acid and nicotinic acid) and aniline-containing (3-aminobenzoic acid and anthranilic acid) monocarboxylates were integrated within defective UiO-66 with this method. Non-defective UiO-66 modified with linkers bearing the same amino groups (2,5-pyridinedicarboxylic acid and 2-aminoterephthalic acid) were prepared by classical post-synthetic ligand exchange (PSE), in order to compare the effect of introducing functionalities at defective sites versus installing them on the backbone. PSDE reduces the porosity of defective UiO-66, but improves both the CO2 uptake and the CO2/N2 selectivity, whereas PSE has no effect on the porosity of non-defective UiO-66, improving the CO2 uptake but leaving selectivity unchanged. Modification of defective UiO-66 with benzoic acid reveals that pore size reduction is the main factor responsible for the observed uptake improvement, whereas the presence of nitrogen atoms in the pores seems to be beneficial for increasing selectivity.</abstract><type>Journal Article</type><journal>Dalton Transactions</journal><volume>48</volume><journalNumber>10</journalNumber><paginationStart>3349</paginationStart><paginationEnd>3359</paginationEnd><publisher/><issnPrint>1477-9226</issnPrint><issnElectronic>1477-9234</issnElectronic><keywords/><publishedDay>31</publishedDay><publishedMonth>12</publishedMonth><publishedYear>2019</publishedYear><publishedDate>2019-12-31</publishedDate><doi>10.1039/C9DT00154A</doi><url/><notes/><college>COLLEGE NANME</college><department>Engineering</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>EEN</DepartmentCode><institution>Swansea University</institution><apcterm/><lastEdited>2019-03-26T14:05:59.6926796</lastEdited><Created>2019-02-14T09:32:43.1310146</Created><path><level id="1">Faculty of Science and Engineering</level><level id="2">School of Engineering and Applied Sciences - Chemical Engineering</level></path><authors><author><firstname>Athanasios</firstname><surname>Koutsianos</surname><order>1</order></author><author><firstname>Ewa</firstname><surname>Kazimierska</surname><order>2</order></author><author><firstname>Andrew</firstname><surname>Barron</surname><orcid>0000-0002-2018-8288</orcid><order>3</order></author><author><firstname>Marco</firstname><surname>Taddei</surname><orcid>0000-0003-2805-6375</orcid><order>4</order></author><author><firstname>Enrico</firstname><surname>Andreoli</surname><orcid>0000-0002-1207-2314</orcid><order>5</order></author></authors><documents><document><filename>0048825-14022019093453.pdf</filename><originalFilename>koutsianos2019.pdf</originalFilename><uploaded>2019-02-14T09:34:53.8100000</uploaded><type>Output</type><contentLength>1767287</contentLength><contentType>application/pdf</contentType><version>Accepted Manuscript</version><cronfaStatus>true</cronfaStatus><embargoDate>2020-02-13T00:00:00.0000000</embargoDate><copyrightCorrect>true</copyrightCorrect><language>eng</language></document></documents><OutputDurs/></rfc1807>
spelling 2019-03-26T14:05:59.6926796 v2 48825 2019-02-14 A new approach to enhancing the CO2 capture performance of defective UiO-66 via post-synthetic defect exchange acd104d55246ee2d03420795510359e9 Ewa Kazimierska Ewa Kazimierska 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 2019-02-14 EEN Zirconium-based metal-organic frameworks (Zr-MOFs) are a subclass of MOFs known for their remarkable stability, especially in the presence of water. This makes them extremely attractive for practical applications, including CO2 capture from industrial emission sources; however, the CO2 adsorption capacity of Zr-MOFs is moderate compared to that of the best performing MOFs reported to date. Functionalization of Zr-MOFs with amino groups has been demonstrated to increase their affinity for CO2. In this work, we assessed the potential of post-synthetic defect exchange (PSDE) as an alternative approach to introduce amino functionalities at missing-cluster defective sites in formic acid modulated UiO-66. Both pyridine-containing (picolinic acid and nicotinic acid) and aniline-containing (3-aminobenzoic acid and anthranilic acid) monocarboxylates were integrated within defective UiO-66 with this method. Non-defective UiO-66 modified with linkers bearing the same amino groups (2,5-pyridinedicarboxylic acid and 2-aminoterephthalic acid) were prepared by classical post-synthetic ligand exchange (PSE), in order to compare the effect of introducing functionalities at defective sites versus installing them on the backbone. PSDE reduces the porosity of defective UiO-66, but improves both the CO2 uptake and the CO2/N2 selectivity, whereas PSE has no effect on the porosity of non-defective UiO-66, improving the CO2 uptake but leaving selectivity unchanged. Modification of defective UiO-66 with benzoic acid reveals that pore size reduction is the main factor responsible for the observed uptake improvement, whereas the presence of nitrogen atoms in the pores seems to be beneficial for increasing selectivity. Journal Article Dalton Transactions 48 10 3349 3359 1477-9226 1477-9234 31 12 2019 2019-12-31 10.1039/C9DT00154A COLLEGE NANME Engineering COLLEGE CODE EEN Swansea University 2019-03-26T14:05:59.6926796 2019-02-14T09:32:43.1310146 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemical Engineering Athanasios Koutsianos 1 Ewa Kazimierska 2 Andrew Barron 0000-0002-2018-8288 3 Marco Taddei 0000-0003-2805-6375 4 Enrico Andreoli 0000-0002-1207-2314 5 0048825-14022019093453.pdf koutsianos2019.pdf 2019-02-14T09:34:53.8100000 Output 1767287 application/pdf Accepted Manuscript true 2020-02-13T00:00:00.0000000 true eng
title A new approach to enhancing the CO2 capture performance of defective UiO-66 via post-synthetic defect exchange
spellingShingle A new approach to enhancing the CO2 capture performance of defective UiO-66 via post-synthetic defect exchange
Ewa Kazimierska
Andrew Barron
Marco Taddei
Enrico Andreoli
title_short A new approach to enhancing the CO2 capture performance of defective UiO-66 via post-synthetic defect exchange
title_full A new approach to enhancing the CO2 capture performance of defective UiO-66 via post-synthetic defect exchange
title_fullStr A new approach to enhancing the CO2 capture performance of defective UiO-66 via post-synthetic defect exchange
title_full_unstemmed A new approach to enhancing the CO2 capture performance of defective UiO-66 via post-synthetic defect exchange
title_sort A new approach to enhancing the CO2 capture performance of defective UiO-66 via post-synthetic defect exchange
author_id_str_mv acd104d55246ee2d03420795510359e9
92e452f20936d688d36f91c78574241d
5cffd1038508554d8596dee8b4e51052
cbd843daab780bb55698a3daccd74df8
author_id_fullname_str_mv acd104d55246ee2d03420795510359e9_***_Ewa Kazimierska
92e452f20936d688d36f91c78574241d_***_Andrew Barron
5cffd1038508554d8596dee8b4e51052_***_Marco Taddei
cbd843daab780bb55698a3daccd74df8_***_Enrico Andreoli
author Ewa Kazimierska
Andrew Barron
Marco Taddei
Enrico Andreoli
author2 Athanasios Koutsianos
Ewa Kazimierska
Andrew Barron
Marco Taddei
Enrico Andreoli
format Journal article
container_title Dalton Transactions
container_volume 48
container_issue 10
container_start_page 3349
publishDate 2019
institution Swansea University
issn 1477-9226
1477-9234
doi_str_mv 10.1039/C9DT00154A
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 - Chemical Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemical Engineering
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description Zirconium-based metal-organic frameworks (Zr-MOFs) are a subclass of MOFs known for their remarkable stability, especially in the presence of water. This makes them extremely attractive for practical applications, including CO2 capture from industrial emission sources; however, the CO2 adsorption capacity of Zr-MOFs is moderate compared to that of the best performing MOFs reported to date. Functionalization of Zr-MOFs with amino groups has been demonstrated to increase their affinity for CO2. In this work, we assessed the potential of post-synthetic defect exchange (PSDE) as an alternative approach to introduce amino functionalities at missing-cluster defective sites in formic acid modulated UiO-66. Both pyridine-containing (picolinic acid and nicotinic acid) and aniline-containing (3-aminobenzoic acid and anthranilic acid) monocarboxylates were integrated within defective UiO-66 with this method. Non-defective UiO-66 modified with linkers bearing the same amino groups (2,5-pyridinedicarboxylic acid and 2-aminoterephthalic acid) were prepared by classical post-synthetic ligand exchange (PSE), in order to compare the effect of introducing functionalities at defective sites versus installing them on the backbone. PSDE reduces the porosity of defective UiO-66, but improves both the CO2 uptake and the CO2/N2 selectivity, whereas PSE has no effect on the porosity of non-defective UiO-66, improving the CO2 uptake but leaving selectivity unchanged. Modification of defective UiO-66 with benzoic acid reveals that pore size reduction is the main factor responsible for the observed uptake improvement, whereas the presence of nitrogen atoms in the pores seems to be beneficial for increasing selectivity.
published_date 2019-12-31T03:53:40Z
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score 10.92735