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Void Space versus Surface Functionalization for Proton Conduction in Metal-Organic Frameworks.

Marvin K Sarango-Ramírez1, Junkil Park2, Jihan Kim2

  • 1Division of Chemistry, Graduate School of Science, Kyoto University, Kitashirakawa-Oiwakecho, Sakyo-ku, Kyoto 606-8502, Japan.

Angewandte Chemie (International Ed. in English)
|May 19, 2021
PubMed
Summary
This summary is machine-generated.

Void space and pore surface functionality are key for proton-conductive metal-organic frameworks (MOFs). Lower porosity MOFs with consistent surface modification exhibit superior proton conductivity, challenging assumptions about pore volume importance.

Keywords:
functionalitymetal-organic frameworkspostsynthetic modificationproton conductivityvoid space

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Area of Science:

  • Materials Science
  • Chemistry
  • Nanotechnology

Background:

  • Proton-conductive metal-organic frameworks (MOFs) are crucial for energy applications.
  • Void space and pore surface functionality are identified as key structural factors influencing proton conductivity.
  • The relative importance of these factors in MOF design remains unclear.

Purpose of the Study:

  • To investigate the impact of void space and pore-surface modification on proton conduction in MOFs.
  • To compare the priority of void space versus surface functionality in designing proton-conductive MOFs.
  • To elucidate the relationship between MOF structure and proton transport efficiency.

Main Methods:

  • Synthesis and characterization of surface-modified isoreticular MOF-74(Ni) series.
  • Systematic variation of porosity while maintaining surface functionality.
  • Measurement of proton conductivity in MOFs impregnated with conducting media.
  • Density functional theory (DFT) calculations to analyze conduction mechanisms.

Main Results:

  • MOFs with lower porosity demonstrated higher proton conductivity compared to those with higher porosity, given the same surface functionality.
  • The amount of conducting medium impregnated was less in lower porosity MOFs, yet conductivity was superior.
  • DFT calculations indicated that strong hydrogen bonding in high-porosity MOFs hinders efficient proton transport.

Conclusions:

  • Void space, specifically lower porosity, is a more critical factor than previously assumed for optimizing proton conductivity in MOFs.
  • Pore-surface modification plays a significant role, but its effectiveness is modulated by the available void space.
  • Design strategies for proton-conductive MOFs should prioritize controlled porosity alongside surface functionalization for enhanced performance.