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J Org Chem ; 79(6): 2591-600, 2014 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-24597593

RESUMO

Nucleophilic ring opening of 23H-[21,23-didehydro-10,15,20-tris(4-methoxycarbonylphenyl)-5-oxaporphyrinato](trifluoroacetato)zinc(II) with various nucleophiles such as alkoxide, amine, thiolate, and enolate gave 19-substituted bilinone zinc complexes, and they were isolated as free base bilinones. An X-ray crystallographic study demonstrated that the product of 5-oxaporphyrin with sodium methoxide was 21H,23H-(4Z,9Z,15Z)-1,21-dihydro-19-methoxy-5,10,15-tris(4-methoxycarbonylphenyl)bilin-1-one with a helicoidal conformation. The structure of the product of 5-oxaporphyrin with an enolate of ethyl acetoacetate was 21H,22H,24H-(4Z,9Z,15Z,19E)-19-(1-ethoxycarbonyl-2-oxopropylidene)-5,10,15-tris(4-methoxycarbonylphenyl)-1,19,21,24-tetrahydrobilin-1-one, with three inner NH groups. The product with SH(-) was also the same tautomer, 21H,22H,24H-19-thioxo-bilin-1-one, with three NH groups, while the products with RO(-), RNH2, and RS(-) nucleophiles were 21H,23H-bilin-1-ones with two inner NH groups. The first-order rate constants of the ring opening reaction of 5-oxaporphyrin with 1 M BnOH and BnSH in toluene at 303 K were 3.0 × 10(-4) and 6.1 × 10(-4) s(-1), respectively. The ratio of the rate of alcohol to thiol was much higher than that with methyl iodide, suggesting that 5-oxaporphyrin reacted as a hard electrophile in comparison to methyl iodide. UV-visible spectra of 19-substituted bilinones in CHCl3 at 298 K showed that the absorption maximum of the lower energy band was red-shifted in increasing order of O-substituted (645 nm), S-substituted (668 nm), N-substituted (699 nm), and C-substituted bilinones (706 nm).


Assuntos
Bilirrubina/análogos & derivados , Bilirrubina/química , Complexos de Coordenação/química , Nitrogênio/química , Oxigênio/química , Porfirinas/química , Enxofre/química , Zinco/química , Cristalografia por Raios X , Conformação Molecular , Estrutura Molecular
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