Bottom-Up Synthesis of Crystalline Covalent Organic Framework Nanosheets, Nanotubes, and Kippah Vesicles: An Odd-Even Effect Induction

Publikation: Beitrag in FachzeitschriftForschungsartikelBeigetragenBegutachtung

Beitragende

  • Kalipada Koner - , Indian Institute of Science Education and Research, Kolkata (Autor:in)
  • Arnab Sadhukhan - , Indian Institute of Science Education and Research, Kolkata (Autor:in)
  • Suvendu Karak - , Indian Institute of Science Education and Research, Kolkata (Autor:in)
  • Himadri Sekhar Sasmal - , Indian Institute of Science Education and Research, Kolkata (Autor:in)
  • Yutaro Ogaeri - , JEOL Ltd. (Autor:in)
  • Yusuke Nishiyama - , JEOL Ltd. (Autor:in)
  • Shuangjie Zhao - , Fakultät Chemie u. Lebensmittelchemie (Autor:in)
  • Miroslav Položij - , Fakultät Chemie u. Lebensmittelchemie, Helmholtz-Zentrum Dresden-Rossendorf (Autor:in)
  • Agnieszka Kuc - , Helmholtz-Zentrum Dresden-Rossendorf (Autor:in)
  • Thomas Heine - , Fakultät Chemie u. Lebensmittelchemie, Helmholtz-Zentrum Dresden-Rossendorf, Yonsei University (Autor:in)
  • Rahul Banerjee - , Indian Institute of Science Education and Research, Kolkata (Autor:in)

Abstract

Few-layer organic nanosheets are becoming increasingly attractive as two-dimensional (2D) materials due to their precise atomic connectivity and tailor-made pores. However, most strategies for synthesizing nanosheets rely on surface-assisted methods or top-down exfoliation of stacked materials. A bottom-up approach with well-designed building blocks would be the convenient pathway to achieve the bulk-scale synthesis of 2D nanosheets with uniform size and crystallinity. Herein, we have synthesized crystalline covalent organic framework nanosheets (CONs) by reacting tetratopic thianthrene tetraaldehyde (THT) and aliphatic diamines. The bent geometry of thianthrene in THT retards the out-of-plane stacking, while the flexible diamines introduce dynamic characteristics into the framework, facilitating nanosheet formation. Successful isoreticulation with five diamines with two to six carbon chain lengths generalizes the design strategy. Microscopic imaging reveals that the odd and even diamine-based CONs transmute to different nanostructures, such as nanotubes and hollow spheres. The single-crystal X-ray diffraction structure of repeating units indicates that the odd-even linker units of diamines introduce irregular-regular curvature in the backbone, aiding such dimensionality conversion. Theoretical calculations shed more light on nanosheet stacking and rolling behavior with respect to the odd-even effects.

Details

OriginalspracheEnglisch
Seiten (von - bis)14475-14483
Seitenumfang9
FachzeitschriftJournal of the American Chemical Society
Jahrgang145
Ausgabenummer26
PublikationsstatusVeröffentlicht - 5 Juli 2023
Peer-Review-StatusJa

Externe IDs

PubMed 37339245
WOS 001016732700001

Schlagworte

Schlagwörter

  • Surface synthesis, Exfoliation