Reaction mechanism of the buffer-catalyzed and substituted [beta]-cyclodextrin-catalyzed hydrolysis of catechol cyclic phosphates.

Bibliographic Details
Main Author: Bokser, Allan David
Other Authors: Raushel, Frank M. (degree committee member.), Sander, Eugene G. (degree committee member.), Wong, Chi-Huey (degree committee member.)
Format: Thesis Book
Language:English
Published: 1987.
Subjects:
Online Access:Link to ProQuest copy
Link to OAKTrust copy

MARC

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049 |a TXAM 
099 |a 1987  |a Dissertation  |a B686 
100 1 |a Bokser, Allan David. 
245 1 0 |a Reaction mechanism of the buffer-catalyzed and substituted [beta]-cyclodextrin-catalyzed hydrolysis of catechol cyclic phosphates. 
264 1 |c 1987. 
300 |a xviii, 218 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 Typescript (photocopy). 
500 |a Vita. 
502 |b Ph. D. in Chemistry  |c Texas A & M University  |d 1987 
504 |a Includes bibliographical references (leaves 194-200). 
520 3 |a The mechanism for the imidazole-catalyzed hydrolysis of catechol cyclic phosphate has been investigated. The Bronsted β-value obtained for the buffer-catalyzed hydrolyses at a 1:1 buffer ratio was 0.41. The Hammett φ-value obtained for the 1:1-[imidazole]: [imidazolium ion] buffer-catalyzed hydrolysis of substituted catechol cyclic phosphate was 1.08. The proton inventory plots for the imidazole-catalyzed hydrolysis of catechol cyclic phosphate at buffer ratios 75:25, 50:50, and 25:75 [imidazole]: [imidazolium] were dome-shaped, linear, and bowl-shaped, respectively. These different proton inventories indicate that the rate determining step of the reaction changes with the [imidazole]: [imidazolium] ratio and, thus, supports a stepwise mechanism for this reaction. An inverse solvent isotope effect for the hydroxide catalyzed hydrolysis of catechol cyclic phosphate (k(D₂O)/k(H₂O) = 1.63) and the decrease in the normal solvent isotope effects for the imidazole-catalyzed hydrolysis of 4-chlorocatechol cyclic phosphate and 4-nitrocatechol cyclic phosphate (k(H₂O)/k(D₂O) = 1.44, 1.83, respectively) further support this stepwise mechanism. Based on the ³¹P-NMR spectra for the β-cyclodextrin and substituted β-cyclodextrin-catalyzed hydrolysis of 4-tert butyl catechol cyclic phosphate, 6, the reaction occurs with inclusion of the 4-tert butyl catechol cyclic phosphate into the cavity of the cyclodextrin followed by the formation of the product. Heptakis-(2,6-dimethoxy)-β-cyclodextrin and heptakis-(2,3,6-trimethoxy)-β-cyclodextrin were poorer catalysts for the hydrolysis of 6 and 6-mono-imidazole β-cyclodextrin was a better catalyst for the hydrolysis of 6 than β-cyclodextrin. The solvent isotope effects, k(H₂O)/k(D₂O), for the β-cyclodextrin-catalyzed and the 6-mono-imidazole β-cyclodextrin-catalyzed hydrolyses of 6 were 1.35 and 2.35, respectively. Based on the proton inventory for the 6-mono-imidazole β-cyclodextrin-catalyzed hydrolysis of 6, the reaction mechanism is similar to that for the simple model study. 
650 0 |a Bioorganic chemistry. 
650 0 |a Catechol. 
650 0 |a Cyclodextrins. 
650 0 |a Enzymes. 
650 4 |a Major chemistry. 
655 7 |a Academic theses  |2 lcgft 
700 1 |a Hogg, John L.,  |e degree supervisor. 
700 1 |a Raushel, Frank M.,  |e degree committee member. 
700 1 |a Sander, Eugene G.,  |e degree committee member. 
700 1 |a Wong, Chi-Huey,  |e degree committee member. 
710 2 |a Texas A & M University,  |e degree granting institution. 
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856 4 1 |u https://hdl.handle.net/1969.1/DISSERTATIONS-26894  |z Link to OAKTrust copy  |t 0 
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