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PMID: 284381 Published · ppublish English Journal Article Research Support, U.S. Gov't, Non-P.H.S.

Do cleavages of amides by serine proteases occur through a stepwise pathway involving tetrahedral intermediates?

Komiyama M, Bender ML

Abstract

The mechanism of the serine protease-catalyzed cleavage of amides (acylation) was examined in terms of the basicity of the functional groups participating in the catalysis. It is proposed that the reaction does not proceed through a stepwise pathway, as opposed to the cleavage of esters and anilides, which start with general base-catalyzed formation of the tetrahedral intermediate followed by its general acid-catalyzed breakdown. Instead, the proton abstracted from the hydroxyl group of the serine by the imidazolyl group of the histidine is donated to the nitrogen atom of the leaving group of the amide before the bond between the carbonyl carbon atom of the amide and the attacking serine oxygen atom is completed. Reactions proceed by a SN2-like reaction through the cooperation of acid catalysis by the imidazolyl cation and nucleophilic attack by the serine. The mechanisms of the enzymatic hydrolyses of anilides and esters proceed through a discrete tetrahedral intermediate, but the enzymatic hydrolyses of amides probably do not.

MeSH Terms
Amides Binding Sites Catalysis Histidine Hydrolysis Kinetics Peptide Hydrolases/metabolism Serine
Chemicals
Amides Serine Histidine Peptide Hydrolases
Authors & Affiliations
2 authors, click to expand affiliations / ORCID
Komiyama M
Bender M L
References (25)
25 references, click to expand
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Article Info
Journal
Proceedings of the National Academy of Sciences of the United States of America
Abbr.
Proc Natl Acad Sci U S A
ISSN
0027-8424
Published
1979-02-00
Pages
557-60
Language
English
Region
United States
NLM ID
7505876
PMCID
PMC382987
Subset
IM
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