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

Abstract

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

Authors:
ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); USDOE Office of Science - Office of Basic Energy Sciences - Scientific User Facilities Division; U.S. Army Research Laboratory - U.S. Army Research Office (ARO)
OSTI Identifier:
1460958
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Science
Additional Journal Information:
Journal Volume: 361; Journal Issue: 6397; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English

Citation Formats

Evans, Austin M., Parent, Lucas R., Flanders, Nathan C., Bisbey, Ryan P., Vitaku, Edon, Kirschner, Matthew S., Schaller, Richard D., Chen, Lin X., Gianneschi, Nathan C., and Dichtel, William R.. Seeded growth of single-crystal two-dimensional covalent organic frameworks. United States: N. p., 2018. Web. doi:10.1126/science.aar7883.
Evans, Austin M., Parent, Lucas R., Flanders, Nathan C., Bisbey, Ryan P., Vitaku, Edon, Kirschner, Matthew S., Schaller, Richard D., Chen, Lin X., Gianneschi, Nathan C., & Dichtel, William R.. Seeded growth of single-crystal two-dimensional covalent organic frameworks. United States. https://doi.org/10.1126/science.aar7883
Evans, Austin M., Parent, Lucas R., Flanders, Nathan C., Bisbey, Ryan P., Vitaku, Edon, Kirschner, Matthew S., Schaller, Richard D., Chen, Lin X., Gianneschi, Nathan C., and Dichtel, William R.. Thu . "Seeded growth of single-crystal two-dimensional covalent organic frameworks". United States. https://doi.org/10.1126/science.aar7883.
@article{osti_1460958,
title = {Seeded growth of single-crystal two-dimensional covalent organic frameworks},
author = {Evans, Austin M. and Parent, Lucas R. and Flanders, Nathan C. and Bisbey, Ryan P. and Vitaku, Edon and Kirschner, Matthew S. and Schaller, Richard D. and Chen, Lin X. and Gianneschi, Nathan C. and Dichtel, William R.},
abstractNote = {Polymerizing monomers into periodic two-dimensional (2D) networks provides structurally precise, layered macromolecular sheets that exhibit desirable mechanical, optoelectrotronic, and molecular transport properties. 2D covalent organic frameworks (COFs) offer broad monomer scope but are generally isolated as powders comprised of aggregated nanometer-scale crystallites. Here we control 2D COF formation using a two-step procedure, in which monomers are added slowly to pre-formed nanoparticle seeds. The resulting 2D COFs are isolated as single-crystalline, micron-sized particles. Transient absorption spectroscopy of the dispersed COF nanoparticles provides two to three orders of magnitude improvement in signal quality relative to polycrystalline powder samples and suggests exciton diffusion over longer length scales than those obtained through previous approaches. These findings will enable a broad exploration of synthetic 2D polymer structures and properties.},
doi = {10.1126/science.aar7883},
url = {https://www.osti.gov/biblio/1460958}, journal = {Science},
issn = {0036-8075},
number = 6397,
volume = 361,
place = {United States},
year = {2018},
month = {6}
}

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