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Orbital Steering in the Catalytic Power of Enzymes: Small Structural Changes with Large Catalytic Consequences
Abstract
Small structural perturbations in the enzyme isocitrate dehydrogenase (IDH) were made in order to evaluate the contribution of precise substrate alignment to the catalytic power of an enzyme. The reaction trajectory of IDH was modified (i) after the adenine moiety of nicotinamide adenine dinucleotide phosphate was changed to hypoxanthine (the 6-amino was changed to 6-hydroxyl), and (ii) by replacing Mg 2+ , which has six coordinating ligands, with Ca 2+ , which has eight coordinating ligands. Both changes make large (10 −3 to 10 −5 ) changes in the reaction velocity but only small changes in the orientation of the substrates (both distance and angle) as revealed by cryocrystallographic trapping of active IDH complexes. The results provide evidence that orbital overlap produced by optimal orientation of reacting orbitals plays a major quantitative role in the catalytic power of enzymes.
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Citations
Cited by
An NMR Perspective on Enzyme Dynamics
Boehr, D. D., Dyson, H. J., & Wright, P. E. (2006) · Chemical Reviews · doi:10.1021/cr050312q · Cited by 458
Improving enzyme properties: when are closer mutations better?
Morley, K. L., & Kazlauskas, R. J. (2005) · Trends in Biotechnology · doi:10.1016/j.tibtech.2005.03.005 · Cited by 438
QM/MM Methods for Biological Systems
Senn, H. M., & Thiel, W. (2006) · Topics in Current Chemistry · doi:10.1007/128_2006_084 · Cited by 428
The allosteric regulation of pyruvate kinase by fructose-1,6-bisphosphate
Jurica, M. S., Mesecar, A., Heath, P. J., Shi, W., Nowak, T., & Stoddard, B. L. (1998) · Structure · doi:10.1016/s0969-2126(98)00021-5 · Cited by 426
Self-citationRatia, K., Saikatendu, K. S., Santarsiero, B. D., Barretto, N., Baker, S. C., Stevens, R. C., & Mesecar, A. D. (2006) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.0510851103 · Cited by 414
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Metadata
- Authors
- Mesecar, A. D., Stoddard, B. L., & Koshland, D. E.
- Venue
- Science
- Published
- 1997-07-11
- Volume
- 277
- Issue
- 5323
- Pages
- 202-206
- ISSN
- 0036-8075 (ISSN-L)
- 1095-9203
- OpenAlex
- W2116243606
- Cited by
- 206
- References
- 0
- FWCI
- 12.68
- Type
- journal article
- Language
- en
- Open access
- closed
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- Mesecar, A. D., Stoddard, B. L., & Koshland, D. E. (1997). Orbital Steering in the Catalytic Power of Enzymes: Small Structural Changes with Large Catalytic Consequences. Science. https://doi.org/10.1126/science.277.5323.202
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Contains information from the Semantic Scholar Academic Graph Datasets, made available under the ODC Attribution License (ODC-BY 1.0).
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