Chemistry and Physics
of
ELSEVIER SCIENCE Chemistry and Physics of Lipids LIPIDS
IRELAND 70 (1994) 43--51
Infrared study of the bilayer stability behavior of binary and
ternary phospholipid mixtures containing unsaturated
phosphatidylethanolamine
Kwan Hon Cheng
Physics Department, Texas Tech University, Box 41051, Lubbock, TX 79409-1051, USA
(Received 7 June 1993; revision received ! November 1993;accepted I November 1993)
Abstract
The bilayer stability of liposomes containing unsaturated phosphatidylethanolamine (PE) has been investigated by
measuring the C~O and CH2 stretching frequencies of the lipids at different lipid compositions and temperatures.
Binary mixtures of 1-palmitoyl-2-oleoylphosphatidyleholine (POPC) and dilinoleoyl-PE (DLPE) are known to exhibit
lamellar liquid crystalline (L,), inverted hexagonal (Hn) and metastable intermediate (I) phases. Abrupt increases in
the C~--O and CH2 stretching frequencies at 65-75 and 90-95% PE, respectively, were found as the PE content of
the DLPE/POPC mixtures was increased from 0 to 100%. These transitions were associated with the La-I and I-HII
phase transitions of the DLPE/POPC mixtures, accordingly. The effects of three lipid perturbants, butylated hydroxy-
toluene (BHT), diacylglyeerol (DG) and cholesterol (CL), on the above L~-I and I-H n transitions were also exam-
ined. All perturbants were found to be effective in shifting the L~-I transition of the DLPC/POPC mixtures to a lower
PE% as detected by the C=O stretching frequency measurements. On the other hand, the perturbants appeared to
eliminate the I-Hn transition of the DLP~POPC mixtures as detected by the CH2 stretching frequency
measurements. The effectiveness of the perturbants in promoting the La-I phase transition of the DLPE/POPC mix-
tures followed the order of DG > BHT > CL. The phase boundaries of this L~-I transition at different lipid and
perturbant compositions were further quantitated by the use of three-dimensional contour plots (Cheng, Chem. and
Phys. Lipids, 60, 119-125 (1991)) of the C~O frequency as a function of DLPE/POPC and perturbant/lipid composi-
tions. It was concluded that the lipid C=O vibrational frequency is a useful and non-invasive parameter for examining
the bilayer stability of liposomes.
Key words: FTIR; Phase transitions; Metastable phases; Bilayer defects
1. Introduction
Under physiological conditions, most unsatur-
ated phosphatidylethanolamine (PE) lipids
undergo first-order temperature-driven lamellar
liquid crystalline (L~) to non-lamellar, or non-
bilayer, inverted hexagonal (Hn) phase transitions
at well-defined temperatures. For the case of
binary mixtures containing unsaturated PE, e.g.,
PE/phosphatidylcholine (PC), composition-driven
L~-Hn transitions can also occur. The tendency
or propensity of the lipids to undergo temperature-
or composition-driven L~-Hu transitions, or the
stability of lipid bilayer, is believed to play a key
role in various membrane-related functions, such
as ion transport [1,2], membrane fusion [3,4] and
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