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Crystal Dynamics in Multi-stimuli-Responsive Entangled Metal-Organic Frameworks.

Prakash Kanoo1,2, Ritesh Haldar3, Sandeep K Reddy1

  • 1Chemistry and Physics of Materials Unit (CPMU), Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR), Jakkur, Bangalore-, 560064, Karnataka, India.

Chemistry (Weinheim an Der Bergstrasse, Germany)
|September 10, 2016
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Flexible metal-organic frameworks (MOFs) show structural changes crucial for sensing. This study details f-MOF-1

Keywords:
breathingcarbon dioxidemetal-organic frameworkspolymorphismselective gas adsorption

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Area of Science:

  • Materials Science
  • Crystallography
  • Chemical Engineering

Background:

  • Understanding solid-state crystal dynamics in flexible metal-organic frameworks (MOFs) is vital for designing advanced materials.
  • Entangled MOFs exhibiting flexibility present challenges in dynamic analysis due to poor single-crystallinity.

Purpose of the Study:

  • To investigate the structural response of a twofold entangled MOF (f-MOF-1) to external stimuli like temperature, pressure, and guest molecules.
  • To elucidate the mechanism behind the selective and gated carbon dioxide (CO2) adsorption in f-MOF-1.
  • To explore the influence of linker functionality on the gate-opening pressure of CO2 adsorption in analogous MOFs.

Main Methods:

  • Detailed experimental studies including crystallographic analysis.
  • Isolation and characterization of distinct desolvated phases (f-MOF-1a and f-MOF-1b).
  • Density Functional Theory (DFT)-based calculations to understand adsorption behavior and inter-net interactions.

Main Results:

  • f-MOF-1 exhibits multiple structural changes, deforming and sliding upon guest removal, leading to two distinct desolvated phases.
  • The two phases, f-MOF-1a (metastable) and f-MOF-1b, display different gated CO2 adsorption profiles.
  • DFT calculations reveal the selective and gated CO2 adsorption mechanism in f-MOF-1b.
  • Modulating linker functionality (e.g., from ethanylene to azo groups) in analogous MOFs tunes the CO2 gate-opening pressure.

Conclusions:

  • The framework of f-MOF-1 is highly responsive to CO2 gas molecules, demonstrating potential for gas separation and sensing applications.
  • Structural flexibility and linker functionality are key factors in controlling guest molecule adsorption in MOFs.
  • The findings provide valuable insights for the rational design of responsive MOFs with tunable properties.