Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 139, Issue 37, Pages 13166-13172Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b07457
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Funding
- BASF SE (Ludwigshafen, Germany)
- King Abdulaziz City for Science and Technology as part of a joint KACST-UC Berkeley collaboration (Center of Excellence for Nanomaterials and Clean Energy Applications)
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
- ShanghaiTech Startup Funding
- Shanghai Science and Technology Committee [17ZR1418600]
- SIP fellowship
- Army Research Office for the Multidisciplinary University Research Initiatives award [WG11NF-15-1-0047]
- Spanish Ministry of Economy and Competitiveness through Ramon y Cajal program
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Developing synthetic methodology to crystallize extended covalent structures has been an important pursuit of reticular chemistry. Here, we report a homogeneous synthetic route for imine covalent organic frameworks (COFs) where crystallites emerge from clear solutions without forming amorphous polyimine precipitates. The key feature of this route is the utilization of tert-butyloxycarbonyl group protected amine building blocks, which are deprotected in situ and gradually nucleate the crystalline framework. We demonstrate the utility of this approach by crystallizing a woven covalent organic framework (COF-112), in which covalent organic threads are interlaced to form a three-dimensional woven framework. The homogeneous imine COF synthesis also enabled the control of nucleation and crystal growth leading to uniform nanocrystals, through microwave-assisted reactions, and facile preparation of oriented thin films.
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