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Water-Based Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal–Organic Frameworks with UiO-66 and MIL-140 Topology

Roberto D’Amato, Anna Donnadio, Mariolino Carta Orcid Logo, Claudio Sangregorio, Davide Tiana, Riccardo Vivani, Marco Taddei Orcid Logo, Ferdinando Costantino

ACS Sustainable Chemistry & Engineering

Swansea University Authors: Mariolino Carta Orcid Logo, Marco Taddei Orcid Logo

Abstract

Reaction of cerium ammonium nitrate and tetrafluoroterephthalic acid in water afforded two new metal–organic frameworks with UiO-66 [F4_UiO-66(Ce)] and MIL-140 [F4_MIL-140A(Ce)] topologies. The two compounds can be obtained in the same experimental conditions, just by varying the amount of acetic ac...

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Published in: ACS Sustainable Chemistry & Engineering
ISSN: 2168-0485 2168-0485
Published: 2018
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URI: https://cronfa.swan.ac.uk/Record/cronfa47916
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spelling 2019-01-03T15:32:09.0830260 v2 47916 2018-12-10 Water-Based Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal–Organic Frameworks with UiO-66 and MIL-140 Topology 56aebf2bba457f395149bbecbfa6d3eb 0000-0003-0718-6971 Mariolino Carta Mariolino Carta true false 5cffd1038508554d8596dee8b4e51052 0000-0003-2805-6375 Marco Taddei Marco Taddei true false 2018-12-10 CHEM Reaction of cerium ammonium nitrate and tetrafluoroterephthalic acid in water afforded two new metal–organic frameworks with UiO-66 [F4_UiO-66(Ce)] and MIL-140 [F4_MIL-140A(Ce)] topologies. The two compounds can be obtained in the same experimental conditions, just by varying the amount of acetic acid used as crystallization modulator in the synthesis. Both F4_UiO-66(Ce) and F4_MIL-140A(Ce) feature pores with size <8 Å, which classifies them as ultramicroporous. Combination of X-ray photoelectron spectroscopy and magnetic susceptibility measurements revealed that both compounds contain a small amount of Ce(III), which is preferentially accumulated near the surface of the crystallites. The CO2 sorption properties of F4_UiO-66(Ce) and F4_MIL-140A(Ce) were investigated, finding that they perform better than their Zr-based analogues. F4_MIL-140A(Ce) displays an unusual S-shaped isotherm with steep uptake increase at pressure <0.2 bar at 298 K. This makes F4_MIL-140A(Ce) exceptionally selective for CO2 over N2: the calculated selectivity, according to the ideal adsorbed solution theory for a 0.15:0.85 mixture at 1 bar and 293 K, is higher than 1900, among the highest ever reported for metal–organic frameworks. The calculated isosteric heat of CO2 adsorption is in the range of 38–40 kJ mol–1, indicating a strong physisorptive character. Journal Article ACS Sustainable Chemistry & Engineering 2168-0485 2168-0485 Carbon dioxide capture; Gas separations; Green synthesis; Metal−organic frameworks; Porous materials 31 12 2018 2018-12-31 10.1021/acssuschemeng.8b03765 Data Access Statement:Crystallographic data presented in this paper can be obtained free of charge from the Cambridge Crystallographic Data Centre under entries CCDC-1855704 and CCDC-1855705 via www.ccdc.cam.ac.uk/data_request/cif. COLLEGE NANME Chemistry COLLEGE CODE CHEM Swansea University 2019-01-03T15:32:09.0830260 2018-12-10T09:17:25.5076702 Faculty of Science and Engineering School of Engineering and Applied Sciences - Uncategorised Roberto D’Amato 1 Anna Donnadio 2 Mariolino Carta 0000-0003-0718-6971 3 Claudio Sangregorio 4 Davide Tiana 5 Riccardo Vivani 6 Marco Taddei 0000-0003-2805-6375 7 Ferdinando Costantino 8 0047916-10122018092501.pdf damato2018.pdf 2018-12-10T09:25:01.5170000 Output 943081 application/pdf Accepted Manuscript true 2019-11-23T00:00:00.0000000 true eng
title Water-Based Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal–Organic Frameworks with UiO-66 and MIL-140 Topology
spellingShingle Water-Based Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal–Organic Frameworks with UiO-66 and MIL-140 Topology
Mariolino Carta
Marco Taddei
title_short Water-Based Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal–Organic Frameworks with UiO-66 and MIL-140 Topology
title_full Water-Based Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal–Organic Frameworks with UiO-66 and MIL-140 Topology
title_fullStr Water-Based Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal–Organic Frameworks with UiO-66 and MIL-140 Topology
title_full_unstemmed Water-Based Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal–Organic Frameworks with UiO-66 and MIL-140 Topology
title_sort Water-Based Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal–Organic Frameworks with UiO-66 and MIL-140 Topology
author_id_str_mv 56aebf2bba457f395149bbecbfa6d3eb
5cffd1038508554d8596dee8b4e51052
author_id_fullname_str_mv 56aebf2bba457f395149bbecbfa6d3eb_***_Mariolino Carta
5cffd1038508554d8596dee8b4e51052_***_Marco Taddei
author Mariolino Carta
Marco Taddei
author2 Roberto D’Amato
Anna Donnadio
Mariolino Carta
Claudio Sangregorio
Davide Tiana
Riccardo Vivani
Marco Taddei
Ferdinando Costantino
format Journal article
container_title ACS Sustainable Chemistry & Engineering
publishDate 2018
institution Swansea University
issn 2168-0485
2168-0485
doi_str_mv 10.1021/acssuschemeng.8b03765
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 - Uncategorised{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Uncategorised
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description Reaction of cerium ammonium nitrate and tetrafluoroterephthalic acid in water afforded two new metal–organic frameworks with UiO-66 [F4_UiO-66(Ce)] and MIL-140 [F4_MIL-140A(Ce)] topologies. The two compounds can be obtained in the same experimental conditions, just by varying the amount of acetic acid used as crystallization modulator in the synthesis. Both F4_UiO-66(Ce) and F4_MIL-140A(Ce) feature pores with size <8 Å, which classifies them as ultramicroporous. Combination of X-ray photoelectron spectroscopy and magnetic susceptibility measurements revealed that both compounds contain a small amount of Ce(III), which is preferentially accumulated near the surface of the crystallites. The CO2 sorption properties of F4_UiO-66(Ce) and F4_MIL-140A(Ce) were investigated, finding that they perform better than their Zr-based analogues. F4_MIL-140A(Ce) displays an unusual S-shaped isotherm with steep uptake increase at pressure <0.2 bar at 298 K. This makes F4_MIL-140A(Ce) exceptionally selective for CO2 over N2: the calculated selectivity, according to the ideal adsorbed solution theory for a 0.15:0.85 mixture at 1 bar and 293 K, is higher than 1900, among the highest ever reported for metal–organic frameworks. The calculated isosteric heat of CO2 adsorption is in the range of 38–40 kJ mol–1, indicating a strong physisorptive character.
published_date 2018-12-31T03:58:08Z
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