期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 28, 期 57, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202201929
关键词
hydrogen bonds; frameworks; molecular reorganization; single crystal to single crystal; supramolecular chemistry
资金
- Australian Research Council [DE170100200, FT210100495]
- Australian Research Council [FT210100495] Funding Source: Australian Research Council
Three isoreticular hydrogen bonded organic frameworks assembled through charge-assisted amidinium center dot center dot center dot carboxylate hydrogen bonds were studied, revealing extreme yet recoverable molecular-level framework reorganization during phase transitions. The water content was found to control the transformations, and the non-porous anhydrous phase showed reversible water sorption through crystal restructuring.
As hydrogen bonded frameworks are held together by relatively weak interactions, they often form several different frameworks under slightly different synthesis conditions and respond dynamically to stimuli such as heat and vacuum. However, these dynamic restructuring processes are often poorly understood. In this work, three isoreticular hydrogen bonded organic frameworks assembled through charge-assisted amidinium center dot center dot center dot carboxylate hydrogen bonds (1(C/C), 1(Si/C) and 1(Si/Si)) are studied. Three distinct phases for 1(C/C) and four for 1(Si/C) and 1(Si/Si) are fully structurally characterized. The transitions between these phases involve extreme yet recoverable molecular-level framework reorganization. It is demonstrated that these transformations are related to water content and can be controlled by humidity, and that the non-porous anhydrous phase of 1(C/C) shows reversible water sorption through single crystal to crystal restructuring. This mechanistic insight opens the way for the future use of the inherent dynamism present in hydrogen bonded frameworks.
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