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Competition between side-chain interactions dictates 2D polymer stacking order.

Alexander K Oanta1, Chloe E Pelkowski1, Michael J Strauss1

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Controlling the stacking of two-dimensional polymers (2DPs) is key for their applications. High zwitterion loading degrades 2DP quality by disrupting polymer stacking, impacting material properties.

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Area of Science:

  • Materials Science
  • Polymer Chemistry
  • Nanotechnology

Background:

  • Two-dimensional polymers (2DPs) are advanced materials with tunable properties.
  • Understanding the factors influencing 2DPs stacking is crucial for optimizing their performance.
  • The role of pore-confined species in dictating 2DP structural integrity requires further investigation.

Purpose of the Study:

  • To investigate how varying amounts of zwitterions within 2DP pores affect material crystallinity and porosity.
  • To elucidate the interplay between zwitterion loading, electrostatic forces, and alkyl chain interactions in directing 2DP stacking.
  • To establish structure-property relationships for zwitterion-modified 2DPs.

Main Methods:

  • Synthesis of 2DPs with controlled zwitterion incorporation.
  • Characterization of 2DP crystallinity and porosity using techniques such as X-ray diffraction and gas adsorption.
  • Analysis of the electrostatic and steric interactions governing 2DP assembly.

Main Results:

  • High loadings of zwitterions within 2DP pores were found to consistently decrease the quality of the 2DP materials.
  • A competitive mechanism between zwitterion-induced electrostatic disruption and alkyl chain stabilization was identified as the primary determinant of 2DP stacking.
  • The composition of the polymer side chains significantly influenced the resulting 2DP crystallinity and porosity.

Conclusions:

  • Zwitterion incorporation, particularly at high concentrations, negatively impacts 2DP structural quality and properties.
  • The stacking behavior of 2DPs is sensitive to the balance of forces between pore-confined species and polymer side chains.
  • Tailoring side chain chemistry is essential for controlling 2DP stacking and achieving desired material characteristics.