Experimental evidence for hydrogen tunneling when the isotopic arrhenius prefactor (A h/A d) is unity

Journal of the American Chemical Society

Volumn 130, Issue 52, 2008, Pages 17632-17633

  Sharma, Sudhir C ^a   Klinman, Judith P ^a  

^a UNIVERSITY OF CALIFORNIA   (United States)

Author keywords

[No Author keywords available]

Indexed keywords

ARRHENIUS; CONDENSED PHASE; DOUBLE MUTANTS; EXPERIMENTAL EVIDENCE; HYDROGEN-TRANSFER REACTIONS; KINETIC ISOTOPE EFFECTS; PREFACTOR; QUANTUM MECHANICAL; SEMICLASSICAL MODEL; SOYBEAN LIPOXYGENASE; TEMPERATURE DEPENDENCE;

ISOTOPES; TUNNELING (EXCAVATION); WIND TUNNELS;

HYDROGEN;

DEUTERIUM; HYDROGEN; ISOTOPE; LIPOXYGENASE; LIPOXYGENASE L 1; LIPOXYGENASE L-1; UNCLASSIFIED DRUG;

CATALYSIS; CATALYST; CRYSTAL STRUCTURE; ENZYME MECHANISM; ROOM TEMPERATURE; SHORT SURVEY; SPECTRAL SENSITIVITY; TEMPERATURE DEPENDENCE; ARTICLE; CHEMISTRY; KINETICS; METABOLISM; TEMPERATURE; THERMODYNAMICS;

DEUTERIUM; HYDROGEN; KINETICS; LIPOXYGENASE; TEMPERATURE; THERMODYNAMICS;

EID: 58849126229     PISSN: 00027863     EISSN: None     Source Type: Journal    
DOI: 10.1021/ja806354w     Document Type: Short Survey

References (24)

1. Bell, R. P. The Tunnel Effect in Chemistry; Chapman and Hall: London; New York, 1980.
2. Swain, C. G.; Stivers, E. C; Reuwer, J. F.; Schaad, L. J. J. Am. Chem. Soc. 1958, 80, 5885.
3. Cha, Y.; Murray, C. J.; Klinman, J. P. Science 1989, 243, 1325.
4. (a) Knapp, M. J.; Rickert, K.; Klinman, J. P. J. Am. Chem. Soc. 2002,124, 3865.
5. (b) Knapp, M. J.; Klinman, J. P Eur. J. Biochem. 2002, 269, 3113.
6. (a) Grant, K. L.; Klinman, J. P. Biochemistry 1989, 28, 6597.
7. (b) Whittaker, M. M.; Ballou, D. P.; Whittaker, J. W. Biochemistry 1998, 37, 8426.
8. (c) Chowdhury, S.; Banerjee, R. J. Am. Chem. Soc. 2000, 122, 5417.
9. (a) Sikorski, R. S.; Wang, L.; Markham, K. A.; Rajagopalan, P. T. R.; Benkovic, S. J.; Kohen, A. J. Am. Chem. Soc. 2004, 126, 4778.
10. (b) Francisco, W. A.; Knapp, M. J.; Blackburn, N. J.; Klinman, J. P. J. Am. Chem. Soc. 2002, 124, 8194.
11. (c) Basran, J.; Sutcliffe, M. J.; Scrutton, N. S. Biochemistry 1999, 38, 3218.
12. (d) Kohen, A.; Cannio, R.; Bartolucci, S.; Klinman, J. P. Nature 1999, 399, 496.
13. Klinman, J. P. Phil. Trans. R. Soc. 2006, B361, 1323.
14. Kuznetsov, A. M.; Ulstrup, J. Can. J. Chem. 1999, 77, 1085.
15. Glickman, M. H.; Klinman, J. P. Biochemistry 1996, 35, 12882.
16. (a) Rickert, K. W.; Klinman, J. P. Biochemistry 1999, 38, 12218.
17. (b) Jonsson, T.; Glickman, M. H.; Sun, S.; Klinman, J. P. J. Am. Chem. Soc. 1996, 118, 10319.
18. Tomchick, D. R.; Phan, P.; Cymborowski, M.; Minor, W.; Holman, T. R. Biochemistry 2001, 40, 7509.
19. Meyer, M. P.; Tomchick, D. R.; Klinman, J. P. Proc. Natl. Acad. Sci. U.S.A. 2008, 105, 1146.
20. The fact that the rate for H transfer is seen in selected mutants to vary very little in relation to WT, while D transfer is impeded, can be understood in the context of a compensating decrease in the force constant for gating that accompanies the increase in donor/acceptor distance. This aspect will be treated in greater detail elsewhere.
21. Wang, L.; Goodey, N. M.; Benkovic, S. J.; Kohen, A. Proc. Natl. Acad. Sci. U.S.A. 2006, 103, 15753.
22. Maglia, G.; Allemann, R. K. J. Am. Chem. Soc. 2003, 125, 13372.
23. Seymour, S. L.; Klinman, J. P. Biochemistry 2002, 41, 8747.
24. Tsai, S. C.; Klinman, J. P. Biochemistry 2001, 40, 2303.