The reaction of diphenylethylenes with boron trifluoride and water

1977 ◽  
Vol 55 (1) ◽  
pp. 85-90 ◽  
Author(s):  
Stanley Bywater ◽  
Denis J. Worsfold

The concentrations have been measured of carbenium ions formed when diphenylethylene and diphenylpropene react with boron trifluoride and water in methylene chloride solution. With both these olefins it appeared necessary that two boron trifluoride molecules should be present for every water molecule to form the carbenium ion. Also the ionic species formed showed a very high degree of ionic dissociation. Diphenylethylene rapidly formed the cyclized dimer, and as a side reaction formed some triphenylmethylcarbenium ions. The diphenylpropene gave a diphenylcarbenium ion that appeared stable, but the accompanying anion was thought to be unstable and rearranged to a more stable form which disrupted the dependences on the concentrations of original reactants.

1984 ◽  
Vol 37 (6) ◽  
pp. 1313 ◽  
Author(s):  
H Becker ◽  
SR Hall ◽  
BW Skelton ◽  
AH White

.A new, metastable phase of lepidopterene, (5,6,11,12-tetrahydro-4b,12[1',2']:6,10b[1",2"]-dibenzenochrysene) (1), has been obtained from methylene chloride solution, exhibiting a luminescence which differs from that of the stable form, having an absorption maximum at 580 nm rather than 560 nm. Single crystal X-ray diffraction determination of the structure of the new phase shows it to be orthorhombic, Pbcn, a 36.75(3), b 7.229(7), c 44.85(3) Ǻ, Z 24, the structure being refined to a residual of 0.065 for 2413 independent 'observed' reflections. Despite the relatively low precision of the determination, it is evident that in the metastable form, the gross molecular disposition is severely distorted. The crystal structure of dimethyllepidopterene (2) has also been determined, and refined by least squares to a residual of 0.041 for 632 'observed' reflections. Crystals are mono- clinic, P21/c, with a 9.607(4), b 11.564(7), c 10.576(6) Ǻ, β 107.72(4), Z 2; the molecules are centrosymmetric. Tetrachlorolepidopterene (31, formed by the dimerization of 1,5-dichloro-9-anthrylmethyl, yields two crystalline forms from xylene and methylene chloride solutions which differ in their crystal exciplex luminescence, showing emission maxima at 590 and 575 nrn respectively. Single- crystal X-ray structure determination confirms that the two crystalline forms, α- and β-, are polymorphs of the same centrosymmetric molecular species. For the α-form, crystals are triclinic, P1 , a 15.374(6), b 9.858(4), c 8.000(4) Ǻ, α 83.98(4), β 83.73(3), γ 71.53(3)°, Z 2, 2138 independent 'observed' reflections being refined to a residual of 0.037; the unit cell contains two independent centrosymmetric molecules. For the β-form, crystals are monoclinic, C2/c, a 11.03(2), b 13.67(2), c 16.32(3) Ǻ, β 1 1 1.13(12)°, Z 4; the residual for 1554 independent reflections was 0.053.


1963 ◽  
Vol 41 (10) ◽  
pp. 2671-2682 ◽  
Author(s):  
B. E. Leggetter ◽  
R. K. Brown

A number of 1,3-oxathiolanes and 1,3-dithiolanes were subjected to reduction in ether solution by lithium aluminum hydride in the presence of either aluminum chloride or boron trifluoride. Both of these Lewis acids not only isomerized 1,3-oxathiolanes but also catalyzed their hydrogenolysis to the hydroxy thioethers. Under the same conditions neither aluminum chloride nor boron trifluoride had any effect upon 1,3-dithiolanes. However, in methylene chloride solution, 1,3-dithiolanes are isomerized by both Lewis acids although their hydrogenolysis was not achieved, probably due to the insolubility of the hydride in methylene chloride.A mechanistic interpretation is discussed to explain the results obtained.


1978 ◽  
Vol 56 (15) ◽  
pp. 2093-2095 ◽  
Author(s):  
Stanley Bywater ◽  
Denis J. Worsfold

SnCl4 and HCl have been found to react with 1,1-diphenylpropene to form a small equilibrium amount of the diphenylethylcarbenium ion. No further reaction is detectable, and the equilibrium between the three reactants may be determined from the uv absorption of the ion. The electrical conductances of the solutions have also been measured. The results are consistent with the formation of the salt of this carbenium ion with the SnCl5− anion. The salt in the concentrations formed in these experiments (ca. 10−5–10−4 M) was nearly all dissociated into free ions in methylene chloride solution. The equilibrium constant for formation of the salt was 2.0 M−2 at −30 °C, and the dissociation constant into ions 4.4 × 10−4 M. The overall heat of reaction to the carbenium ion salt was 8.8 kcal, most of which is attributed to the initial formation of the undissociated salt.


1967 ◽  
Vol 45 (20) ◽  
pp. 2403-2409 ◽  
Author(s):  
S. Brownstein

Tetrabutylammonium halides react with one or more molecules of boron trifluoride or phosphorus pentafluoride at low temperature in dilute methylene chloride solution. Rapid, frequently concentration dependent equilibria occur in the nonideal solutions. The products isolated upon evaporation of solvent may not be those present in the dilute solutions. Usually a disproportionation occurs to yield BF4− or PF6−. With the exception of B2F7−, no complex ions involving fluorine bridging were found in solution or in the reaction products.


1979 ◽  
Vol 57 (1) ◽  
pp. 119-127 ◽  
Author(s):  
Dennis G. Garratt ◽  
Pierre Beaulieu

The reaction of 2,4-dinitrobenzenesulphenyl chloride with eight alkyl 1,3-disubstituted allenes in methylene chloride solution has been investigated. In contrast to earlier reports, attack by sulphur is found to occur exclusively at the central allenic carbon. The direction of approach of sulphenyl chloride leads preferentially to the formation of the E isomers in accord with the concept of steric approach control. The ratio of E to Z alkene is found to increase as the bulk of the substituent group cis to the arylthio group increases. We observe, however, very little regioselectivity with respect to which of the mutually perpendicular π bonds of the allene system is attacked, suggesting the presence of an effective mechanism for transmission of inductive effects to the more distant double bond.


1996 ◽  
Vol 74 (11) ◽  
pp. 2331-2339 ◽  
Author(s):  
Sean R. Klopfenstein ◽  
Constanze Kluwe ◽  
Kristin Kirschbaum ◽  
Julian A. Davies

The binuciear palladium(I) complex, [Pd2Cl2(μ-dppm)2] (dppm = bis(diphenylphosphino)methane), has been shown to react with bis(diethylamino)acetylene, Et2NC≡CNEt2, in methylene chloride solution to yield two isolable products, the known methylene-bridged complex, [Pd2Cl2(μ-CH2)(μ-dppm)2], and hexakis(diethylamino)benzene, C6(NEt2)6, both of which have been characterized crystallographically. The source of the bridging methylene group in [Pd2Cl2(μ-CH2)(μ-dppm)2] has been shown to be the methylene chloride solvent. A mechanism that accounts for the formation of the two isolable products is proposed. The complex, [Pd2Cl2(μdmpm)2] (dmpm = bis(dimethylphosphino)methane), was similarly found to react with Et2NC≡NEt2 in methylene chloride solution to yield [Pd2Cl2(μ-CH2)(μ-dmpm)2], which was identified spectroscopically. Key words: acetylene, palladium, cyclooligomerization, aminoacetylene, hexakis(diethylamino)benzene.


1968 ◽  
Vol 46 (12) ◽  
pp. 2147-2157 ◽  
Author(s):  
R. J. Gillespie ◽  
J. S. Hartman

1H and 19F n.m.r. studies of BF3 adducts of some simple methyl ketones in methylene chloride solution have led to the following conclusions. (1) Only 1:1 adducts are formed which are not appreciably dissociated. (2) The down-field shifts of the proton resonances caused by complexation with BF3 are essentially independent of the ketone and depend only on the distance of the proton from the carbonyl group. (3) BF3 exchange is rapid on the n.m.r. time scale at room temperature, but the exchange process can be slowed sufficiently by lowering the temperature that separate signals due to free and complexed species can be observed. (4) Collapse of the 10B−11B isotope shift with increasing temperature showed that a second chemical exchange process, which exchanges fluorine among boron atoms, occurs in addition to the process of rapid breaking and re-forming of donor–acceptor bonds. A possible mechanism for this fluorine scrambling reaction is discussed.


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