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Direct Structural Identification of Gas Induced Gate‐Opening Coupled with Commensurate Adsorption in a Microporous Metal–Organic Framework

Journal Article · · Chemistry - A European Journal
 [1];  [2];  [3];  [2];  [4];  [2]
  1. Department of Chemistry and Chemical Biology Rutgers University Piscataway New Jersey 08854 USA, Fundamental and Computational Science Directorate Pacific Northwest National Laboratory Richland Washington 99352 USA
  2. Department of Chemistry and Chemical Biology Rutgers University Piscataway New Jersey 08854 USA
  3. Department of Geosciences Stony Brook University Stony Brook New York 11794 USA, Physics Department Yeshiva University New York NY 10016 USA
  4. Department of Geosciences Stony Brook University Stony Brook New York 11794 USA
Abstract

Gate‐opening is a unique and interesting phenomenon commonly observed in flexible porous frameworks, where the pore characteristics and/or crystal structures change in response to external stimuli such as adding or removing guest molecules. For gate‐opening that is induced by gas adsorption, the pore‐opening pressure often varies for different adsorbate molecules and, thus, can be applied to selectively separate a gas mixture. The detailed understanding of this phenomenon is of fundamental importance to the design of industrially applicable gas‐selective sorbents, which remains under investigated due to the lack of direct structural evidence for such systems. We report a mechanistic study of gas‐induced gate‐opening process of a microporous metal–organic framework, [Mn(ina) 2 ] (ina=isonicotinate) associated with commensurate adsorption, by a combination of several analytical techniques including single crystal X‐ray diffraction, in situ powder X‐ray diffraction coupled with differential scanning calorimetry (XRD‐DSC), and gas adsorption–desorption methods. Our study reveals that the pronounced and reversible gate opening/closing phenomena observed in [Mn(ina) 2 ] are coupled with a structural transition that involves rotation of the organic linker molecules as a result of interaction of the framework with adsorbed gas molecules including carbon dioxide and propane. The onset pressure to open the gate correlates with the extent of such interaction.

Sponsoring Organization:
USDOE
Grant/Contract Number:
FG02-08ER46491
OSTI ID:
1400463
Journal Information:
Chemistry - A European Journal, Journal Name: Chemistry - A European Journal Journal Issue: 33 Vol. 22; ISSN 0947-6539
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English

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