Pseudo-5-Fold-Symmetrical Ligand Drives Geometric Frustration in Porous Metal-Organic and Hydrogen-Bonded Frameworks

Frederik Haase*, Gavin A. Craig, Mickaële Bonneau, Kunihisa Sugimoto, Shuhei Furukawa*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

17 Scopus citations

Abstract

Reticular framework materials thrive on designability, but unexpected reaction outcomes are crucial in exploring new structures and functionalities. By combining "incompatible"building blocks, we employed geometric frustration in reticular materials leading to emergent structural features. The combination of a pseudo-C5-symmetrical organic building unit based on a pyrrole core with a C4-symmetrical copper paddlewheel synthon led to three distinct frameworks by tuning the synthetic conditions. The frameworks show structural features typical for geometric frustration: self-limiting assembly, internally stressed equilibrium structures, and topological defects in the equilibrium structure, which manifested in formation of a hydrogen-bonded framework, distorted and broken secondary building units, and dangling functional groups, respectively. The influence of geometric frustration on the CO2 sorption behavior and the discovery of a new secondary building unit shows geometric frustration can serve as a strategy to obtain highly complex porous frameworks.

Original languageEnglish (US)
Pages (from-to)13839-13845
Number of pages7
JournalJournal of the American Chemical Society
Volume142
Issue number32
DOIs
StatePublished - Aug 12 2020

Bibliographical note

Funding Information:
F.H. is grateful to the Japan Society for the Promotion of Science (JSPS) for Post-Doctoral Fellowships. The authors acknowledge the iCeMS Analysis Center for access to analytical facilities. The authors also acknowledge the anonymous reviewer's detailed suggestion for the discussion of nets.

Publisher Copyright:
Copyright © 2020 American Chemical Society.

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry
  • Biochemistry
  • Colloid and Surface Chemistry

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