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Solvation causes two-dimensional covalent organic frameworks (2D COFs) to shift their layer stacking from AA to quasi-AB structures. This solvent-induced rearrangement is common in 2D COFs and impacts their properties.

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Area of Science:

  • Materials Science
  • Chemistry
  • Crystallography

Background:

  • Layer-stacking structures are prevalent in two-dimensional covalent organic frameworks (2D COFs).
  • The structural behavior of solvated 2D COFs remains largely unexplored compared to their solvent-free counterparts.

Purpose of the Study:

  • To investigate and determine the in situ structures of solvated 2D COFs.
  • To understand the structural differences between solvated and dried 2D COFs.
  • To explore the universality of solvent-induced structural changes in 2D COFs.

Main Methods:

  • In situ determination of solvated 2D COF structures.
  • Powder X-ray diffraction (PXRD) data analysis.
  • Computational modeling including density functional theory (DFT) and Pawley refinement.

Main Results:

  • Solvated 2D COFs exhibit significant interlayer shifting, forming quasi-AB-stacking structures, distinct from the AA-stacking in dried states.
  • Solvent interactions weaken inter-layer attraction, facilitating this structural rearrangement.
  • DFT calculations confirm the energetic preference for quasi-AB stacking in solvated COFs.
  • This phenomenon was observed across four different crystalline 2D COFs, indicating universality.

Conclusions:

  • Solvation induces a universal interlayer stacking rearrangement in 2D COFs from AA to quasi-AB.
  • These findings necessitate a re-evaluation of 2D COF structures in solvated states.
  • The solvent-induced structural changes open new avenues for COF applications in wet conditions.