Z theor BioL (1989) 137, 171-189
Space-filling Effects of Inert Solutes as Probes for the Detection
and Study of Substrate-mediated Conformational Changes by
Enzyme Kinetics: Theoretical Considerations
DOUGLAS A. BERGMAN AND DONALD J. WINZORt
Department of Biochemistry, University of Queensland, St. Lucia,
Queensland 4067, Australia
(Received 8 August 1988)
From expressions derived for the space-filling effects of small inert solutes on kinetic
parameters for univalent enzymes undergoing isomerizations that are substrate-
induced and pre-existing, it is concluded that experimental observation of an
enhanced maximal velocity in the presence of inert solute can only reflect the
existence of the former type of conformational change; and that the isomerization
must be governed by a relatively small equilibrium constant. Similar conclusions
apply to multivalent enzymes exhibiting Michaelis-Menten kinetics. Extension of
the theory, to provide quantitative expressions for multivalent enzymes has made
possible the numerical simulation of thermodynamic non-ideality effects on systems
conforming with the Monod and Koshland models of allostery. In that regard the
simulated Scatchard plots for the two models differ sufficiently in form to suggest
that detailed examination of the space-filling effects of small solutes on the kinetics
of an allosteric enzyme may, under favourable circumstances, allow identification
of the appropriate allosteric mechanism. Finally, these considerations of thermody-
namic non-ideality in relation to the kinetics of allosteric enzymes have revealed
formal similarities between the consequences of space-filling by inert solutes and
the specific effects of allosteric activators or inhibitors. Attention is drawn to the
possible implications of this observation in relation to the functioning of allosteric
enzymes in vivo, where catalytic performance may be modified by factors no more
specific than the ability of unrelated solutes to occupy space in the highly concen-
trated cellular environment.
1. Introduction
Despite the fact that protein isomerization, be it pre-existing (Monod et al., 1965)
or ligand-induced (Koshland et al., 1966), is frequently invoked as the molecular
interaction responsible for many allosteric effects, there is very little direct evidence
for the equilibrium co-existence of different conformational states of an enzyme or
protein. Furthermore, in the few instances where substrate- or effector-mediated
changes in protein conformation have been observed (e.g. Perutz et al., 1964; Gerhact
& Schachman, 1968; Oberfelder et al., 1984a, b), assignment of the isomerization
equilibria as ligand-induced or pre-existing has remained uncertain. This indecision
t To whom all correspondence should be addressed at Department of Biochemistry, University of
Queensland, St. Lucia, QId. 4067, Australia.
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0022-5193/89/060171 + 19 $03.00/0 © 1989 Academic Press Limited