The molecular code for hemoglobin allostery revealed by linking the thermodynamics and kinetics of quaternary structural change. 1. Microstate linear free energy relations

Biochemistry
Robert A GoldbeckDavid S Kliger

Abstract

A novel model linking the thermodynamics and kinetics of hemoglobin's allosteric (R --> T) and ligand binding reactions is applied to photolysis data for human HbCO. To describe hemoglobin's kinetics at the microscopic level of structural transitions and ligand-binding events for individual [ij]-ligation microstates ((ij)R --> (ij)T, (ij)R + CO --> ((i)(+1))(k)R, and (ij)T + CO --> ((i)(+1))(k)T), the model calculates activation energies, (ij)DeltaG(++), from previously measured cooperative free energies of the equilibrium microstates (Huang, Y., and Ackers, G. K. (1996) Biochemistry 35, 704-718) by using linear free energy relations ((ij)DeltaG(++) - (01)DeltaG(++) = alpha[(ij)DeltaG - (01)DeltaG], where the parameter alpha, describing the variation of activation energy with reaction energy perturbation, can depend on the natures of both the reaction and the perturbation). The alpha value measured here for the allosteric dynamics, 0.21 +/- 0.03, corresponds closely to values observed previously, strongly suggesting that the thermodynamic microstate energies directly underlie the allosteric kinetics (as opposed to the alpha((ij)DeltaG(RT)) serving merely as arbitrary fitting parameters). Besides systematizing the study of hemog...Continue Reading

References

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Jan 3, 1992·Science·G K AckersM A Daugherty
May 29, 2000·Biophysical Journal·R M EsquerraD S Kliger
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Jun 27, 2002·Journal of the American Chemical Society·Robert A GoldbeckDavid S Kliger
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Citations

Aug 23, 2008·The Journal of Physical Chemistry. B·Ami D PatelBrian M Hoffman
Apr 16, 2005·Annual Review of Pharmacology and Toxicology·William M Atkins
Jan 25, 2006·Proceedings of the National Academy of Sciences of the United States of America·Robert A GoldbeckRaymond M Esquerra
Dec 22, 2005·Journal of Molecular Biology·Janina KneippThomas G Spiro
Jun 30, 2016·Biochemistry·Raymond M EsquerraRobert A Goldbeck
Jul 20, 2016·Organic & Biomolecular Chemistry·Hans-Jörg Schneider
Mar 3, 2007·Analytical Biochemistry·Edward DeMollAusten F Riggs
Jan 21, 2006·The Journal of Biological Chemistry·Gary K Ackers, Jo M Holt
Aug 9, 2017·Chemistry : a European Journal·Karine BaudetClaude Piguet
Jun 28, 2021·Current Opinion in Structural Biology·Hyun Sun ChoPhilip Anfinrud

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