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Biophys J, January 2001, p. 271-279, Vol. 80, No. 1
Department of Biochemistry, Health Sciences Centre, McMaster University, Hamilton, Ontario, Canada
The energetics of phospholipid aggregation depend on the
apparent water-accessible apolar surface area (ASAap),
ordering effects of the chains, and headgroup interactions. We quantify
the enthalpy and entropy of these interactions separately. For that
purpose, the thermodynamics of micelle formation of
lysophosphatidylcholines (LPCs, chains C10,
C12, C14, and C16) and
diacylphosphatidylcholines (DAPCs, chains C5,
C6, and C7) are studied using isothermal
titration calorimetry. The critical micelle concentration (CMC) values
are 90, 15, and 1.9 mM (C5-C7-DAPC) and 6.8, 0.71, 0.045, and 0.005 mM (LPCs). The group contributions per methylene
of 
G0 = 
3.1 kJ/mol and
CP = 57 J/(mol · K) for LPCs agree with literature data on hydrocarbons and amphiphiles.
An apparent deviation of DAPCs (2.5 kJ/mol, 45 J/(mol · K)) is
due to an intramolecular interaction between the two chains, burying
20% of the surface. The chain/chain interaction enthalpies in a
micelle core are by ~2 kJ/(mol) per methylene group more favorable
than in bulk hydrocarbons. We conclude that the impact of the chain
conformation and packing on the interaction enthalpy is very
pronounced. It serves to explain a variety of effects reported on
membrane binding. Interactions within the water-accessible region show
considerable H, but almost no
G0. The heat capacity changes suggest about
three methylene groups (ASAap 
100 Å2)
per LPC remain exposed to water in a micelle (DAPC: 2 CH2/70 Å2).
Biophys J, January 2001, p. 271-279, Vol. 80, No. 1
© 2001 by the Biophysical Society 0006-3495/01/01/271/09 $2.00
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