By Bernard Pullman (auth.), Bernard Pullman (eds.)
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Additional resources for Catalysis in Chemistry and Biochemistry Theory and Experiment: Proceedings of the Twelfth Jerusalem Symposium on Quantum Chemistry and Biochemistry held in Jerusalem, Israel, April 2–4, 1979
COMPUTATIONAL DETAILS ALL the caLcuLations were carried out with the ab initio SCF moLecuLar orbitaL method (19), using a pseudopotentiaL to repLace the core eLectrons of the atoms (20-21). The method and the gaussian basis sets used have been presented in detaiLs in our previous papers (16,17). The vaLence orbitaL basis sets are of doubLe zeta quaLity, so as to insure enough fLexibiLity in the description of the intermoLecuLar compLexes. A set of diffuse p functions has been added when necessary to describe anions as discussed in detaiLs in reference (16).
1555-1560. EFFICIENCY AND MECHANISM IN INTRAMOLECULAR CATALYSIS Anthony J. Kirby University Chemical Laboratory, Cambridge CB2 lEW, UK The potential efficiency of intramolecular catalysis, as measured by the effective concentration of the catalytic' group, depends strongly on the mechanism. Nucleophilic catalysis can be very efficient indeed, but intramolecular general base, and probably general acid catalysis also, are intrinsically much less efficient. These generalisations are relevant to our understanding of the efficiency of catalysis by enzymes.
Angles a,S DI1I~ Effective Concn. 7 o . 7 -0 The most reactive compound in this series shows extraordinary reactivity: under conditions where ordinary amides have half-lives of hundreds of years, dialkylmaleamic acids have half-lives of less than one second (Kirby and Lancaster) We are thus dealing with simple reactions going at rates comparable with those of some related enzyme catalysed reactions. It is highly significant, therefore, that the mechanisms of intramolecular catalysis change with increasing reactivity.
Catalysis in Chemistry and Biochemistry Theory and Experiment: Proceedings of the Twelfth Jerusalem Symposium on Quantum Chemistry and Biochemistry held in Jerusalem, Israel, April 2–4, 1979 by Bernard Pullman (auth.), Bernard Pullman (eds.)