Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 141, Issue 50, Pages 19728-19735Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b08815
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Funding
- Army Research Office [W911NF-15-1-0447]
- National Science Foundation Graduate Research Fellowship [DGE-1324585]
- National Science Foundation [DMREF-1629383]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- National Institute of Biomedical Imaging and Bioengineering of the National Institutes of Health [F32EB021859]
- National Institutes of Health
- NSF Graduate Research Fellowship [DGE-1842165]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF ECCS-1542205]
- MRSEC program at the Materials Research Center [NSF DMR-1720139]
- Keck Foundation
- State of Illinois
- International Institute for Nanotechnology (IIN)
- NCI CCSG [P30 CA060553]
- 3M graduate research fellowship
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The synthesis of periodic two-dimensional (2D) polymers and characterization of their optoelectronic behaviors are challenges at the forefront of polymer chemistry and materials science. Recently, we showed that layered 2D polymers known as 2D covalent organic frameworks (COFs) can be synthesized as single crystals by preparing COF particles as colloidal suspensions. Here we expand this approach from the condensation of boronic acids and catechols to the dehydrative trimerization of polyboronic acids. The resulting boroxine-linked colloids are the next class of 2D COFs to be obtained as single-crystalline particles, as demonstrated here for four 2D COFs and one 3D COF. Colloidal stabilization enables detailed structural analysis by synchrotron X-ray diffraction and high-resolution transmission electron microscopy. Solution fluorescence spectroscopy revealed that the COF crystallites are highly emissive compared to their respective monomer solutions. Excitation-emission matrix fluorescence spectroscopy indicated that the origin of this enhanced emission can be attributed to through-space communication of chromophores between COF sheets. These observations will motivate the development of colloidal COF systems as a platform to organize functional aromatic systems into precise and predictable assemblies with emergent properties.
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