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Seeded growth of single-crystal two-dimensional covalent organic frameworks

Journal Article · · Science
 [1];  [2];  [1];  [3];  [1];  [1];  [4];  [5];  [2];  [1]
  1. Department of Chemistry, Northwestern University, Evanston, IL 60208, USA.
  2. Department of Chemistry, Northwestern University, Evanston, IL 60208, USA., Department of Materials Science and Engineering, Northwestern University, Evanston, IL 60208, USA., Department of Biomedical Engineering, Northwestern University, Evanston, IL 60208, USA.
  3. Department of Chemistry, Northwestern University, Evanston, IL 60208, USA., Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University, Ithaca, NY 14853, USA.
  4. Department of Chemistry, Northwestern University, Evanston, IL 60208, USA., Center for Nanoscale Materials, Argonne National Laboratory, Argonne, IL 60439, USA.
  5. Department of Chemistry, Northwestern University, Evanston, IL 60208, USA., Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, IL 60439, USA.

Polymerization of monomers into periodic two-dimensional networks provides structurally precise, layered macromolecular sheets that exhibit desirable mechanical, optoelectronic, and molecular transport properties. Two-dimensional covalent organic frameworks (2D COFs) offer broad monomer scope but are generally isolated as powders comprising aggregated nanometer-scale crystallites. We found that 2D COF formation could be controlled using a two-step procedure in which monomers are added slowly to preformed nanoparticle seeds. The resulting 2D COFs are isolated as single-crystalline, micrometer-sized particles. Transient absorption spectroscopy of the dispersed COF nanoparticles revealed improvement in signal quality by two to three orders of magnitude relative to polycrystalline powder samples, and suggests exciton diffusion over longer length scales than those obtained through previous approaches. These findings should enable a broad exploration of synthetic 2D polymer structures and properties.

Sponsoring Organization:
USDOE
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1459055
Alternate ID(s):
OSTI ID: 1460958
Journal Information:
Science, Journal Name: Science Journal Issue: 6397 Vol. 361; ISSN 0036-8075
Publisher:
American Association for the Advancement of Science (AAAS)Copyright Statement
Country of Publication:
United States
Language:
English

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