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Control over Phase Transformations in a Family of Flexible Double Diamondoid Coordination Networks through Linker Ligand Substitution
[Image: see text] In this work, we present the first metal–organic framework (MOF) platform with a self-penetrated double diamondoid (ddi) topology that exhibits switching between closed (nonporous) and open (porous) phases induced by exposure to gases. A crystal engineering strategy, linker ligand...
Autores principales: | , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10173379/ https://www.ncbi.nlm.nih.gov/pubmed/37181677 http://dx.doi.org/10.1021/acs.chemmater.3c00334 |
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author | Koupepidou, Kyriaki Nikolayenko, Varvara I. Sensharma, Debobroto Bezrukov, Andrey A. Shivanna, Mohana Castell, Dominic C. Wang, Shi-Qiang Kumar, Naveen Otake, Ken-ichi Kitagawa, Susumu Zaworotko, Michael J. |
author_facet | Koupepidou, Kyriaki Nikolayenko, Varvara I. Sensharma, Debobroto Bezrukov, Andrey A. Shivanna, Mohana Castell, Dominic C. Wang, Shi-Qiang Kumar, Naveen Otake, Ken-ichi Kitagawa, Susumu Zaworotko, Michael J. |
author_sort | Koupepidou, Kyriaki |
collection | PubMed |
description | [Image: see text] In this work, we present the first metal–organic framework (MOF) platform with a self-penetrated double diamondoid (ddi) topology that exhibits switching between closed (nonporous) and open (porous) phases induced by exposure to gases. A crystal engineering strategy, linker ligand substitution, was used to control gas sorption properties for CO(2) and C3 gases. Specifically, bimbz (1,4-bis(imidazol-1-yl)benzene) in the coordination network X-ddi-1-Ni ([Ni(2)(bimbz)(2)(bdc)(2)(H(2)O)](n), H(2)bdc = 1,4-benzenedicarboxylic acid) was replaced by bimpz (3,6-bis(imidazol-1-yl)pyridazine) in X-ddi-2-Ni ([Ni(2)(bimpz)(2)(bdc)(2)(H(2)O)](n)). In addition, the 1:1 mixed crystal X-ddi-1,2-Ni ([Ni(2)(bimbz)(bimpz)(bdc)(2)(H(2)O)](n)) was prepared and studied. All three variants form isostructural closed (β) phases upon activation which each exhibited different reversible properties upon exposure to CO(2) at 195 K and C3 gases at 273 K. For CO(2), X-ddi-1-Ni revealed incomplete gate-opening, X-ddi-2-Ni exhibited a stepped isotherm with saturation uptake of 3.92 mol·mol(–1), and X-ddi-1,2-Ni achieved up to 62% more gas uptake and a distinct isotherm shape vs the parent materials. Single-crystal X-ray diffraction (SCXRD) and in situ powder X-ray diffraction (PXRD) experiments provided insight into the mechanisms of phase transformation and revealed that the β phases are nonporous with unit cell volumes 39.9, 40.8, and 41.0% lower than the corresponding as-synthesized α phases, X-ddi-1-Ni-α, X-ddi-2-Ni-α, and X-ddi-1,2-Ni-α, respectively. The results presented herein represent the first report of reversible switching between closed and open phases in ddi topology coordination networks and further highlight how ligand substitution can profoundly impact the gas sorption properties of switching sorbents. |
format | Online Article Text |
id | pubmed-10173379 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-101733792023-05-12 Control over Phase Transformations in a Family of Flexible Double Diamondoid Coordination Networks through Linker Ligand Substitution Koupepidou, Kyriaki Nikolayenko, Varvara I. Sensharma, Debobroto Bezrukov, Andrey A. Shivanna, Mohana Castell, Dominic C. Wang, Shi-Qiang Kumar, Naveen Otake, Ken-ichi Kitagawa, Susumu Zaworotko, Michael J. Chem Mater [Image: see text] In this work, we present the first metal–organic framework (MOF) platform with a self-penetrated double diamondoid (ddi) topology that exhibits switching between closed (nonporous) and open (porous) phases induced by exposure to gases. A crystal engineering strategy, linker ligand substitution, was used to control gas sorption properties for CO(2) and C3 gases. Specifically, bimbz (1,4-bis(imidazol-1-yl)benzene) in the coordination network X-ddi-1-Ni ([Ni(2)(bimbz)(2)(bdc)(2)(H(2)O)](n), H(2)bdc = 1,4-benzenedicarboxylic acid) was replaced by bimpz (3,6-bis(imidazol-1-yl)pyridazine) in X-ddi-2-Ni ([Ni(2)(bimpz)(2)(bdc)(2)(H(2)O)](n)). In addition, the 1:1 mixed crystal X-ddi-1,2-Ni ([Ni(2)(bimbz)(bimpz)(bdc)(2)(H(2)O)](n)) was prepared and studied. All three variants form isostructural closed (β) phases upon activation which each exhibited different reversible properties upon exposure to CO(2) at 195 K and C3 gases at 273 K. For CO(2), X-ddi-1-Ni revealed incomplete gate-opening, X-ddi-2-Ni exhibited a stepped isotherm with saturation uptake of 3.92 mol·mol(–1), and X-ddi-1,2-Ni achieved up to 62% more gas uptake and a distinct isotherm shape vs the parent materials. Single-crystal X-ray diffraction (SCXRD) and in situ powder X-ray diffraction (PXRD) experiments provided insight into the mechanisms of phase transformation and revealed that the β phases are nonporous with unit cell volumes 39.9, 40.8, and 41.0% lower than the corresponding as-synthesized α phases, X-ddi-1-Ni-α, X-ddi-2-Ni-α, and X-ddi-1,2-Ni-α, respectively. The results presented herein represent the first report of reversible switching between closed and open phases in ddi topology coordination networks and further highlight how ligand substitution can profoundly impact the gas sorption properties of switching sorbents. American Chemical Society 2023-04-27 /pmc/articles/PMC10173379/ /pubmed/37181677 http://dx.doi.org/10.1021/acs.chemmater.3c00334 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Koupepidou, Kyriaki Nikolayenko, Varvara I. Sensharma, Debobroto Bezrukov, Andrey A. Shivanna, Mohana Castell, Dominic C. Wang, Shi-Qiang Kumar, Naveen Otake, Ken-ichi Kitagawa, Susumu Zaworotko, Michael J. Control over Phase Transformations in a Family of Flexible Double Diamondoid Coordination Networks through Linker Ligand Substitution |
title | Control over
Phase Transformations in a Family of
Flexible Double Diamondoid Coordination Networks through Linker Ligand
Substitution |
title_full | Control over
Phase Transformations in a Family of
Flexible Double Diamondoid Coordination Networks through Linker Ligand
Substitution |
title_fullStr | Control over
Phase Transformations in a Family of
Flexible Double Diamondoid Coordination Networks through Linker Ligand
Substitution |
title_full_unstemmed | Control over
Phase Transformations in a Family of
Flexible Double Diamondoid Coordination Networks through Linker Ligand
Substitution |
title_short | Control over
Phase Transformations in a Family of
Flexible Double Diamondoid Coordination Networks through Linker Ligand
Substitution |
title_sort | control over
phase transformations in a family of
flexible double diamondoid coordination networks through linker ligand
substitution |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10173379/ https://www.ncbi.nlm.nih.gov/pubmed/37181677 http://dx.doi.org/10.1021/acs.chemmater.3c00334 |
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