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Robust Barium Phosphonate Metal–Organic Frameworks Synthesized under Aqueous Conditions


Salmeia, Khalifah A; Dolabella, Simone; Parida, Dambarudhar; Frankcombe, Terry J; Afaneh, Akef T; Cordova, Kyle E; Al-Maythalony, Bassem; Zhao, Shanyu; Civioc, Romain; Marashdeh, Ali; Spingler, Bernhard; Frison, Ruggero; Neels, Antonia (2021). Robust Barium Phosphonate Metal–Organic Frameworks Synthesized under Aqueous Conditions. ACS Materials Letters, 3(7):1010-1015.

Abstract

The design and discovery of three-dimensional crystalline metal–organic frameworks (MOFs) from linkers with phosphonate coordinating groups and even alkaline earth metals is largely undeveloped. Herein, we report a strategy for realizing new, stable, and robust barium phosphonate MOFs, termed Empa-1 and Empa-2. The two-dimensional (2D) Empa-1 or three-dimensional (3D) Empa-2 could be realized by way of systematically modulating the ratio of Ba2+ with a tetratopic phosphonate-based linker that was crafted to incorporate nitrogen-rich triazine units bridged by a fixed piperazine core. In addition to this synthetic approach, temperature-dependent synchrotron-radiation powder X-ray diffraction analysis demonstrated that the 2D Empa-1 undergoes an irreversible phase transition upon heating and subsequent dehydration to form the 3D Empa-2. Given the presence of uncoordinated phosphonic acid moieties within the structure of 3D Empa-2, the CO2 sorption capabilities are reported. We believe our ability to link the alkaline earth metal barium with a novel tetratopic phosphonate linker, as evidenced by the robust structures of Empa-1 and -2, paves the way for further exploration and discovery of new crystalline, porous frameworks with greater structural diversity, stability, and wide-scale practical applicability.

Abstract

The design and discovery of three-dimensional crystalline metal–organic frameworks (MOFs) from linkers with phosphonate coordinating groups and even alkaline earth metals is largely undeveloped. Herein, we report a strategy for realizing new, stable, and robust barium phosphonate MOFs, termed Empa-1 and Empa-2. The two-dimensional (2D) Empa-1 or three-dimensional (3D) Empa-2 could be realized by way of systematically modulating the ratio of Ba2+ with a tetratopic phosphonate-based linker that was crafted to incorporate nitrogen-rich triazine units bridged by a fixed piperazine core. In addition to this synthetic approach, temperature-dependent synchrotron-radiation powder X-ray diffraction analysis demonstrated that the 2D Empa-1 undergoes an irreversible phase transition upon heating and subsequent dehydration to form the 3D Empa-2. Given the presence of uncoordinated phosphonic acid moieties within the structure of 3D Empa-2, the CO2 sorption capabilities are reported. We believe our ability to link the alkaline earth metal barium with a novel tetratopic phosphonate linker, as evidenced by the robust structures of Empa-1 and -2, paves the way for further exploration and discovery of new crystalline, porous frameworks with greater structural diversity, stability, and wide-scale practical applicability.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Scopus Subject Areas:Physical Sciences > General Chemical Engineering
Physical Sciences > Biomedical Engineering
Physical Sciences > General Materials Science
Language:English
Date:5 July 2021
Deposited On:24 Aug 2021 09:26
Last Modified:26 Mar 2024 02:37
Publisher:American Chemical Society (ACS)
ISSN:2639-4979
OA Status:Green
Publisher DOI:https://doi.org/10.1021/acsmaterialslett.1c00275
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  • : Project TitleDual X-ray Wavelength Single-Crystal Diffractometer