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Enzymatic H-Transfer Requires Vibration-Driven Extreme Tunneling
Abstract
Enzymatic breakage of the substrate C-H bond by Methylophilus methyltrophus (sp. W3A1) methylamine dehydrogenase (MADH) has been studied by stopped-flow spectroscopy. The rate of reduction of the tryptophan tryptophylquinone (TTQ) cofactor has a large kinetic isotope effect (KIE = 16.8 +/- 0.5), and the KIE is independent of temperature. Analysis of the temperature dependence of C-H bond breakage revealed that extreme (ground state) quantum tunneling is responsible for the transfer of the hydrogen nucleus. Reaction rates are strongly dependent on temperature, indicating thermally induced, vibrational motion drives the H-transfer reaction. The data provide direct experimental evidence for enzymatic bond breakage by extreme tunneling driven by vibrational motion of the protein scaffold. The results demonstrate that classical transition state theory and its tunneling derivatives do not adequately describe this enzymatic reaction.
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Cited by
Electrostatic Basis for Enzyme Catalysis
Warshel, A., Sharma, P. K., Kato, M., Xiang, Y., Liu, H., & Olsson, M. H. M. (2006) · Chemical Reviews · doi:10.1021/cr0503106 · Cited by 1,444
Q UANTUM M ECHANICAL M ETHODS FOR E NZYME K INETICS
Gao, J., & Truhlar, D. G. (2002) · Annual Review of Physical Chemistry · doi:10.1146/annurev.physchem.53.091301.150114 · Cited by 733
A 21st century revisionist's view at a turning point in enzymology
Nagel, Z. D., & Klinman, J. P. (2009) · Nature Chemical Biology · doi:10.1038/nchembio.204 · Cited by 294
Dynamical Contributions to Enzyme Catalysis: Critical Tests of A Popular Hypothesis
Olsson, M. H. M., Parson, W. W., & Warshel, A. (2006) · Chemical Reviews · doi:10.1021/cr040427e · Cited by 289
Environmentally coupled hydrogen tunneling: Linking catalysis to dynamics
Knapp, M. J., & Klinman, J. P. (2002) · European Journal of Biochemistry · doi:10.1046/j.1432-1033.2002.03022.x · Cited by 281
Metadata
- Authors
- Basran, J., Sutcliffe, M. J., & Scrutton, N. S.
- Venue
- Biochemistry
- Publisher
- American Chemical Society (ACS)
- Published
- 1999-02-18
- Volume
- 38
- Issue
- 10
- Pages
- 3218-3222
- ISSN
- 0006-2960 (ISSN-L)
- 1520-4995
- OpenAlex
- W2121890116
- Cited by
- 246
- References
- 0
- FWCI
- 9.97
- Type
- journal article
- Language
- en
- Open access
- closed
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- Basran, J., Sutcliffe, M. J., & Scrutton, N. S. (1999). Enzymatic H-Transfer Requires Vibration-Driven Extreme Tunneling. Biochemistry. https://doi.org/10.1021/bi982719d
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