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Abstract
The heterolinker zeolitic imidazolate framework, ZIF-60 (Zn(Im)1.5(mIm)0.5), and its previously unreported analogues with formulas ranging between Zn(Im)1.79(4)(mIm)0.21(4) and Zn(Im)1.93(1)(mIm)0.07(1) (where Im is imidazolate and mIm is 2-methylimidazolate) have been synthesized, and their structural response to guest exchange and high pressure is probed by single crystal X-ray diffraction. Guest exchange prompts phase transitions between large-pore (I4/mmm) and intermediate and narrow-pore phases (P42/nmc), where the degree of contraction depends on the guest species and the mIm content of the framework. Structural flexibility in the frameworks with noninteger ligand ratios has been probed to 7 GPa in pressure-transmitting media of N,N-diethylformamide (DEF) and methanol/ethanol (MeOH/EtOH). Pressure-induced adsorption of guests promotes gate-opening in both media to ∼1 GPa. In DEF, the framework undergoes an isostructural phase transition at 2.03 GPa, corresponding to desorption of the guest from the pores. In MeOH/EtOH, the framework undergoes a re-entrant phase transition corresponding to adsorption and desorption of the guest, which is facilitated by the smaller size of MeOH/EtOH media. Two previously unreported ZIFs, denoted as ZIF-GIS-Im/mIm and ZIF-GME-Im/mIm, were also synthesized.
Original language | English |
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Pages (from-to) | 5179-5192 |
Number of pages | 14 |
Journal | Crystal Growth and Design |
Volume | 24 |
Issue number | 12 |
Early online date | 29 May 2024 |
DOIs | |
Publication status | Published - 19 Jun 2024 |
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Anomalous Structural Response in Porous Framework Materials
Moggach, S. (Investigator 01) & Keppert, C. (Investigator 02)
ARC Australian Research Council
1/11/22 → 30/10/25
Project: Research
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Fill it, Squeeze it, Crush it: Extreme Gas Uptake in Microporous Materials
Moggach, S. (Investigator 01)
ARC Australian Research Council
1/10/20 → 30/09/24
Project: Research