Ru(0)-catalysed cross-dimerisation and -trimerisation give a series of di- and triheteroaryl compounds cross-linked by π-conjugated trienyl groups. Their photochemical behaviour is studied using UV-visible absorption spectra, fluorescence emission spectra, and TD-DFT calculations. The cross-trimer prepared from 2,5-dialkynylthiophene with 2 equiv. of 2-butadienylpyridine shows a longer wavelength shift in the absorption maximum than the cross-trimer prepared from dialkynylbenzene with 1-phenylbutadiene. The solvent effect and the TD-DFT calculations suggest that the planarity of the π-conjugated system contributes more than spontaneous polarization. Namely, in the 5-membered thiophene ring, the conjugated trienyl group extends in the same plane (dihedral angle: -4.0°) as the thienyl group, whereas in the 6-membered benzene ring, the planarity is reduced due to steric hindrance (dihedral angle: -24.1°). Thus, the cross-trimers with a 5-membered heteroaryl centre contribute to longer wavelengths of absorption and fluorescence emission due to the increased planarity of the conjugated trienyl groups.
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http://dx.doi.org/10.1039/d3ob00207a | DOI Listing |
Chem Commun (Camb)
July 2024
Department of Applied Chemistry, Graduate School of Engineering, Tokyo University of Agriculture and Technology, 2-24-16 Nakacho, Koganei, Tokyo 184-8588, Japan.
Conjugated and non-conjugated polyenes are important substructures and are often found in biologically active compounds and natural products. Their preparation often needs multiple steps or iterative reactions and as a result, they have poor step economies. In this feature article, we show a new methodology to prepare these substructures by combinations of cross-dimerisation giving borylated polyenes and subsequent cross-coupling reactions.
View Article and Find Full Text PDFOrg Biomol Chem
March 2024
Department of Applied Chemistry, Graduate School of Technology, Tokyo University of Agriculture and Technology, 2-24-16 Nakacho, Koganei, Tokyo 184-8588, Japan.
New direct access to conjugated tetraenes has been achieved. A Ru(0)-catalysed reaction of 1,3-enynes with 1,3-dienes gives 1,3,5,7-octatetraene derivatives by formal regioselective insertion of the alkynyl group of 1,3-enynes into the terminal C-H bond in 1,3-dienes. With a silyl substituent on the alkynyl side in 1,3-enynes, the reaction regioselectively proceeds to give the linear cross-dimerisation product having the silyl group at the internal position.
View Article and Find Full Text PDFOrg Biomol Chem
May 2023
Department of Applied Chemistry, Tokyo University of Agriculture and Technology, 2-24-16 Nakacho, Koganei, Tokyo 184-8588, Japan.
Ru(0)-catalysed cross-dimerisation and -trimerisation give a series of di- and triheteroaryl compounds cross-linked by π-conjugated trienyl groups. Their photochemical behaviour is studied using UV-visible absorption spectra, fluorescence emission spectra, and TD-DFT calculations. The cross-trimer prepared from 2,5-dialkynylthiophene with 2 equiv.
View Article and Find Full Text PDFChem Commun (Camb)
August 2019
Department of Applied Chemistry, Tokyo University of Agriculture and Technology, 2-24-16 Nakacho, Koganei, Tokyo 184-8588, Japan.
A series of borylated conjugated trienes and skipped dienes is prepared by Ru-catalysed cross-dimerisation using alkynyl-, dienyl-, and vinyl boronates. These products are used as synthetic building blocks for polyene substructures by subsequent Pd-catalysed cross-coupling in a one-pot vessel without deprotection.
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