ArticleJournal of physical organic chemistry2010
On the Origin of the Chemical Barrier and Tunneling in Enzymes.
Article in Journal of physical organic chemistry, 2010. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 7 papers.
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Who cites it
7 citing papers in PubMed.
- Computational Studies of Catalytic Loop Dynamics inThe journal of physical chemistry. B · 2019Article
- A Biophysical Perspective on Enzyme Catalysis.Biochemistry · 2019Article
- Carbon Acidity in Enzyme Active Sites.Frontiers in bioengineering and biotechnology · 2019Article
- Path Sampling Methods for Enzymatic Quantum Particle Transfer Reactions.Methods in enzymology · 2016Review
- Dynamics and dissipation in enzyme catalysis.Proceedings of the National Academy of Sciences of the United States of America · 2011Article
- Temperature dependence of the kinetic isotope effects in thymidylate synthase. A theoretical study.Journal of the American Chemical Society · 2011Article
- Enzymatic transition states, transition-state analogs, dynamics, thermodynamics, and lifetimes.Annual review of biochemistry · 2011Review
Corrections and comments
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Authors and funding
3 authors.
Funding
Abstract
This paper presents both a review of some recent results from our group and experimental groups, and some new theoretical results all of which are helping to form a more physically rigorous picture of the process of enzymatic catalysis. A common classical picture of enzymatic catalysis is the transition state tight binding model. Schwartz and Schramm1 have recently argued from both theoretical and experimental results that this picture is incorrect. We now investigate what the nature of barriers might be in enzymatic reactions, and what this viewpoint might imply for tunneling in a hydrogen transfer enzyme. For lactate dehydrogenase we conclude that the enzymes role in catalysis is at least partially to hunt through configuration space for those configurations that minimize chemical free energy barriers. Those configurations do not seem to be stable basins on the free energy surface, and in fact the overall free energy barrier to reaction may well largely be due to this stochastic hunt - both probabilistically and energetically. We suggest further computations to test this hypothesis.
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Registered trials
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