Pergamon
Tetrahedron 54 (1998) 997-1004
TETRAHEDRON
Synthesis and X-Ray Crystallographic Study of 6,12-
Epiiminodibenzo[b,]][1,5]diazocines
Pedro Molina,* Antonio Arques, Alberto T~trraga, Maria del Rosario Ob6n
Departamentode Qufmica Org~ica, Facuitadde Qufmica,Universidadde Murcia,
Campusde Espinardo, E-30071Murcia,Spain
Concepci6n Foces-Foces*
Departamentode Cristalograffa,Institutode Qufmica-Ffsica 'Rocasolano', CSIC,Serrano 119,E-28006Madrid, Spain
Nadine Jagerovic and Jos~ Elguero
Instituto de Qufmica M&lica,CSIC,Juan de la Cierva3, E-28006Madrid, Spain
Received 13 October 1997; revised 10 November 1997; accepted 13 November 1997
Abstract:Seven 6,12-epiiminodibenzo[bJ][1,51diazocines 2 with different substituents at position 13 have
been prepared from o-(triphenylphosphoranylideneamino)benzaldehyde I and the corresponding alipha-
tic and aromatic primary amines in yields ranging from 40 to 80%. The molecular and crystal structures
of componds 2d (R = 4 H3C-C6H 4) and 2e (R = 4 H3CO-C6H4) have been determined by X-Ray analy-
sis. Compound 2d crystallizes as a racemate while compound 2e crystallizes as a unique enantiomer
(absolute configuration R,R). © 1997ElsevierScienceLtd. All rightsreserved.
Although iminophosphorane 1, available by Staudinger reaction between o-azidobenzaldehyde and trip-
henylphosphine, t contains the two reactive groups for an aza Wittig reaction, it has been reported that 1 itself
undergoes neither intra- nor intermolecular aza Wittig reactions. 2 This lack of reactivity has been attributed to
the formation of a resonance-stabilized chelate-ring involving the iminophosphorane and formyl groups.
We have found that iminophosphorane 1 reacts with primary amines (benzylamine, picolylamine, ferro-
H
t a, R = C6Hs-CH 2 (46%)
~ C H O R.NH 2 ~ N . ~ b, R=Fc-CH2(42%)
c, R = 3-CsH4N-CH2 (28%)
d, R = 4 H3C-C6I-I 4 (50%)
v "N=PPh3 e, R = 4 H3CO-C6H 4 (40%)
!
H f, R = 4 CI-C61-14 (80%)
1 2 g, R = 4 Br-C6I-I4(52%)
Scheme 1
cenylmethylamine 3 and anilines) in ethanol at room temperature in the presence of catalytic amounts of acetic
acid to give the tricyclic compounds 2 containing the dibenzo[bJ][1,5]diazocine ring system in yields ranging
from 40 to 80% (Scheme 1). The main interest of these compounds lies in their close analogy with Tr6ger's
bases .4-7
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