Regiochemical and stereochemical studies of cationic pi-cyclizations.

Bibliographic Details
Main Author: Puckett, Paul Malcolm
Other Authors: Newcomb, Martin E. (degree committee member.)
Format: Thesis Book
Language:English
Published: 1982.
Subjects:
Online Access:Link to ProQuest Copy
Link to OAKTrust copy
ProQuest, Abstract

MARC

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099 |a 1982  |a Dissertation  |a P977 
100 1 |a Puckett, Paul Malcolm 
245 1 0 |a Regiochemical and stereochemical studies of cationic pi-cyclizations. 
264 1 |c 1982. 
300 |a xi, 104 leaves :  |b illustrations ;  |c 29 cm 
336 |a text  |b txt  |2 rdacontent 
337 |a unmediated  |b n  |2 rdamedia 
338 |a volume  |b nc  |2 rdacarrier 
500 |a "Major subject: Chemistry." 
500 |a Typescript (photocopy). 
500 |a Vita. 
502 |b Ph. D. in Philosophy  |c Texas A & M University  |d 1982 
504 |a Includes bibliographical references (leaves 100-103). 
520 3 |a Cationic (pi)-cyclization of allenyl alcohols 10a,b and allenyl ketones 11a,b provided evidence that the mode of ring closure of (gamma)-allenyl cationic systems is strongly dependent on the substitution pattern of the allene. Cationic (pi)-cyclization of unsubstituted (gamma)-allenyl systems (11a and 12a) gave only decalin-type products resulting from reaction at the terminal carbon of the allene. The substituted (gamma)-allenyl systems (11b and 12b) gave only hydrindane-type products resulting from reaction at the central carbon of the allene. A general rationale for the regioselectivity of these cyclizations results observed with (gamma)-allenyl systems is developed based upon consideration of orbital overlap as determined from molecular models, and of the effect of alkyl substituents on electrophilic addition to allenes. Cationic (pi)-cyclization of several related cyclohexenyl (53, 54, 56, 57, 58, 59, and 60) and cyclopentenyl (61, 62, 63, and 65) systems provided evidence on the most favored transition state for these stereoselective spirocyclic ring closures. The stereoselectivity induced by cyclohexenyl systems is greater than that of cyclopentenyl systems. Addition of a methyl grop adjacent to the forming spirocyclic center reduces stereoselectivity. Addition of a methyl group to the double bond to form a (delta)-E-olefin increases stereoselectivity in allylic alcohol initiated cyclizations. Addition of a methyl adjacent to the forming spirocyclic center when it is incorporated on a (delta)-E-olefin changes the regioselectivity of the reaction in the case of allylic alcohol initiated cyclizations (but leads to complex mixtures in enone initiated cyclizations). 
650 0 |a Allene. 
650 0 |a Bicyclic compounds  |x Analysis. 
650 0 |a Cations. 
650 0 |a Ring formation (Chemistry) 
650 4 |a Chemistry 
655 7 |a Academic theses  |2 lcgft 
700 1 |a Harding, Kenn E.,  |e degree supervisor. 
700 1 |a Newcomb, Martin E.,  |e degree committee member. 
710 2 |a Texas A & M University,  |e degree granting institution. 
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