Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 1, Issue 42, Pages 13171-13178Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c3ta12515g
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Funding
- Corporate Strategic Research in ExxonMobil Research and Engineering
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Previous work demonstrated the ability of a trace amount of pyridine to stabilize Covalent Organic Frameworks (COF)-5 and -10 in humid air. Pyridine was found to form a mixture of Lewis and Bronsted B-[4] Py-B complexes in addition to the un-complexed B-[3] sites in the framework structures. Further research has shown that higher doses of pyridine convert all remaining B-[3] in COF-5/-10 to Lewis B-[4] and bring about the total and irreversible structural decomposition of COF-5 and COF-10. The results suggest that the accumulated strain in the five-member rings of COF-5/-10 resulting from the formation of tetrahedrally-distorted B-[4] sites at high pyridine loadings, may explain the decomposition of these structures. Alternatively, COF-1 is unstable to exposure to humid air at all pyridine loadings tried, but is not unstable to high doses of pyridine. Whereas the same tetrahedrally-distorted B-[4] sites are formed in COF-1, in this case the six-membered B3O3 ring can accommodate the accumulated ring strain and retain an ordered structure. A thorough solid state NMR and molecular dynamics investigation has led to a new proposed stabilization mechanism in humid air based on the formation of Bronsted B-[4].
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