Journal
CHEMISTRY OF MATERIALS
Volume 31, Issue 4, Pages 1359-1369Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.8b04734
Keywords
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Funding
- European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie [641887]
- European Research Council [647755, 716472]
- Research Foundation Flanders (FWO) [G083016N, 12R1217N, 1501618N, G.0962.13, AKUL/15/15-G0H0816N]
- KU Leuven [C32/16/019]
- Research Board of Ghent University (BOF)
- FWO
- Slovenian Research Agency [P1-0021, N1-0079]
- KU Leuven Research Fund [C14/15/053, OT/12/059]
- Hercules foundation [HER/11/14]
- European Research Council under the European Union's Seventh Framework Programme (FP/2007-2013)/ERC Grant [307523]
- European Research Council (ERC) [647755, 716472] Funding Source: European Research Council (ERC)
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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.
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