Active role of methanol in post-synthetic linker exchange in the metal–organic framework UiO-66
- Author
- Joao Marreiros, Chiara Caratelli, Julianna Hajek (UGent) , Andraž Krajnc, Guillaume Fleury, Bart Bueken, Dirk E. De Vos, Gregor Mali, Maarten B. J. Roeffaers, Veronique Van Speybroeck (UGent) and Rob Ameloot
- Organization
- Project
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- DYNPOR (First principle molecular dynamics simulations for complex chemical transformations in nanoporous materials)
- Abstract
- UiO-66 is known as one of the most robust metal organic framework materials. Nevertheless, UiO-66 has also been shown to undergo postsynthetic exchange of structural linkers with surprising ease in some solvents. To date, the exchange mechanism has not yet been fully elucidated. Here, we show how time-resolved monitoring grants insight into the selected case of exchanging 2-aminoterephthalate into UiO-66 in methanol. Analysis of both the solid and liquid phases, complemented by computational insights, revealed the active role of methanol in the creation and stabilization of dangling linkers. Similar to monocarboxylate defects that can be introduced during UiO-66 synthesis, such dangling linkers undergo fast exchange. The presence of missing-linker or missing-cluster defects at the start of the exchange process was shown to have no considerable impact on the equilibrium composition. After the exchange process, the incoming 2-aminoterephthalate and remaining terephthalate linkers were distributed homogeneously in the framework for the typical submicron size of UiO-66 crystallites.
- Keywords
- Materials Chemistry, General Chemistry, General Chemical Engineering
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Citation
Please use this url to cite or link to this publication: http://hdl.handle.net/1854/LU-8616465
- MLA
- Marreiros, Joao, et al. “Active Role of Methanol in Post-Synthetic Linker Exchange in the Metal–Organic Framework UiO-66.” CHEMISTRY OF MATERIALS, vol. 31, no. 4, 2019, pp. 1359–69, doi:10.1021/acs.chemmater.8b04734.
- APA
- Marreiros, J., Caratelli, C., Hajek, J., Krajnc, A., Fleury, G., Bueken, B., … Ameloot, R. (2019). Active role of methanol in post-synthetic linker exchange in the metal–organic framework UiO-66. CHEMISTRY OF MATERIALS, 31(4), 1359–1369. https://doi.org/10.1021/acs.chemmater.8b04734
- Chicago author-date
- Marreiros, Joao, Chiara Caratelli, Julianna Hajek, Andraž Krajnc, Guillaume Fleury, Bart Bueken, Dirk E. De Vos, et al. 2019. “Active Role of Methanol in Post-Synthetic Linker Exchange in the Metal–Organic Framework UiO-66.” CHEMISTRY OF MATERIALS 31 (4): 1359–69. https://doi.org/10.1021/acs.chemmater.8b04734.
- Chicago author-date (all authors)
- Marreiros, Joao, Chiara Caratelli, Julianna Hajek, Andraž Krajnc, Guillaume Fleury, Bart Bueken, Dirk E. De Vos, Gregor Mali, Maarten B. J. Roeffaers, Veronique Van Speybroeck, and Rob Ameloot. 2019. “Active Role of Methanol in Post-Synthetic Linker Exchange in the Metal–Organic Framework UiO-66.” CHEMISTRY OF MATERIALS 31 (4): 1359–1369. doi:10.1021/acs.chemmater.8b04734.
- Vancouver
- 1.Marreiros J, Caratelli C, Hajek J, Krajnc A, Fleury G, Bueken B, et al. Active role of methanol in post-synthetic linker exchange in the metal–organic framework UiO-66. CHEMISTRY OF MATERIALS. 2019;31(4):1359–69.
- IEEE
- [1]J. Marreiros et al., “Active role of methanol in post-synthetic linker exchange in the metal–organic framework UiO-66,” CHEMISTRY OF MATERIALS, vol. 31, no. 4, pp. 1359–1369, 2019.
@article{8616465,
abstract = {{UiO-66 is known as one of the most robust metal organic framework materials. Nevertheless, UiO-66 has also been shown to undergo postsynthetic exchange of structural linkers with surprising ease in some solvents. To date, the exchange mechanism has not yet been fully elucidated. Here, we show how time-resolved monitoring grants insight into the selected case of exchanging 2-aminoterephthalate into UiO-66 in methanol. Analysis of both the solid and liquid phases, complemented by computational insights, revealed the active role of methanol in the creation and stabilization of dangling linkers. Similar to monocarboxylate defects that can be introduced during UiO-66 synthesis, such dangling linkers undergo fast exchange. The presence of missing-linker or missing-cluster defects at the start of the exchange process was shown to have no considerable impact on the equilibrium composition. After the exchange process, the incoming 2-aminoterephthalate and remaining terephthalate linkers were distributed homogeneously in the framework for the typical submicron size of UiO-66 crystallites.}},
author = {{Marreiros, Joao and Caratelli, Chiara and Hajek, Julianna and Krajnc, Andraž and Fleury, Guillaume and Bueken, Bart and De Vos, Dirk E. and Mali, Gregor and Roeffaers, Maarten B. J. and Van Speybroeck, Veronique and Ameloot, Rob}},
issn = {{0897-4756}},
journal = {{CHEMISTRY OF MATERIALS}},
keywords = {{Materials Chemistry,General Chemistry,General Chemical Engineering}},
language = {{eng}},
number = {{4}},
pages = {{1359--1369}},
title = {{Active role of methanol in post-synthetic linker exchange in the metal–organic framework UiO-66}},
url = {{http://doi.org/10.1021/acs.chemmater.8b04734}},
volume = {{31}},
year = {{2019}},
}
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