Sonication induced sheet formation at the air–water interface†
K. S. Satheeshkumar and R. Jayakumar*
Bio Organic Laboratory, Central Leather Research Institute, Adyar, Chennai 600 020, India
Received (in Cambridge, UK) 15th July 2002, Accepted 20th August 2002
First published as an Advance Article on the web 9th September 2002
A hydrophobic pentadecapeptide, AGAAAA-
GAVVGGLGG (1), part of the prion sequence PrP
(106-127), on fresh aqueous dissolution takes a mixture of
random and sheet conformations which forms a stable
monolayer with a high b-sheet content when compressed at
the air–water interface. This also develops into a kinetically
stabilized b-sheet structure on sonication.
The secondary structure conversion of the prion protein in the
normal form (PrP
c
) into the abnormal form (PrP
sc
) is reported to
be a cause of several human and animal diseases, such as
Creutzfeldt–Jacob disease, Gerstmann–Straussler–Scheinker
syndrome, fatal familial insomnia, sheep scrapie, and bovine
spongiform encephalopathy.
1
PrP
c
has high a-helix and low b-
sheet content
2
in contrast to PrP
sc
, which is rich in b-sheets.
3,4
The reason for this conformational transition is still completely
unknown despite numerous investigations.
5
In this work, we
have shown that peptide 1 on ultrasonic treatment and
compression at the air–water interface forms a stable b-sheet
assembly. Insoluble or sparingly soluble polypeptides and
proteins which form monolayers at the air–liquid interface are
very applicable as models for biological systems to study
structural transitions and orientation effects due to ‘molecular
crowding’.
6–9
The sequence of the peptide used in this study is AGAAAA-
GAVVGGLGG (1), which corresponds to H1 of human prion
protein (residues 113-127). Peptide 1 was prepared by a solid
phase method using Boc chemistry. The purity and composition
were determined by amino acid analysis and were identified by
MALDI-TOF MS analysis. Peptide 1 forms a stable film at the
air–water interface. Fig. 1 shows a pressure–area isotherm for
peptide 1. It is seen that the isotherm of peptide 1 is of the liquid
expanded type (85 Å
2
) indicating the fairly rigid nature of the
film. The value of the molecular area of the monolayer can be
directly evaluated from the intersection of the x-axis with the
tangent line of the isotherm at the onset of the condensed phase
of the film, and is found to be 30 Å
2
per molecule. The collapse
pressure is in the region of 28 mN m
21
. The film formed by
peptide 1 could be transferred to a quartz plate by y-type
(vertical) deposition with a transfer ratio around 0.95. The
circular dichroism (CD) spectrum of the transferred film (20
layers) is shown in the inset of Fig. 1. It is found that the peptide
1 solution spread at the air–water interface results in mono-
layers containing predominant sheet conformation, as shown by
the negative CD at 220 nm and the crossover at 213 nm. This
indicates a profound effect of oriented molecular crowding on
b-sheet assembly.
The CD spectrum of peptide 1 in PBS at pH 7.4, (Fig. 2; curve
a) exhibits a mixture of random, helix, sheet and turn
conformations. The sheet content is ~ 30 %. Peptide 1 solution
in vitro must be incubated for several days at ~ 37 °C and under
basic conditions (pH 10.6) in order to build a significant b-sheet
content. The CD spectrum of incubated protofibrils is given in
the ESI.† On sonication it is known to produce energy rich
vapour–liquid interfaces in the liquid with shear force (cavita-
tion effect). We thought it would be worth investigating the
effect of sonication on the conformation of peptide 1. To our
surprise we found that sonication leads to kinetically stabilized
b-sheet formation.
The CD spectrum of peptide 1 in PBS at pH 7.4 is shown in
Fig. 2 (curve a). The peptide solution was sonicated and the CD
spectrum was recorded at 30 s intervals (Fig. 2, curves a to d).
It is inferred from this study that upon sonication the sheet
conformation predominates. This may be due to a highly
energetic cavitational effect, which leads to interfacial effects
on the aggregates. The plot of % sheet structure versus
sonication time is shown in the inset of Fig. 2. It is tacit that the
sheet structure of peptide 1 increases with sonication time. This
† Electronic supplementary information (ESI) available: CD spectra and
table of secondary structure motifs of peptide 1. See http://www.rsc.org/
suppdata/cc/b2/b206886a/
Fig. 1 Surface area–pressure isotherm for peptide 1. Inset: Circular
dichroism (CD) spectrum of a 20 layer film of peptide 1.
Fig. 2 CD spectra of peptide 1 in PBS at pH 7.4 and at different sonication
time intervals: (a) 0 s, (b) 30 s, (c) 60 s, (d) 90 s. Inset: Plot of % sheet
structure versus sonication time. % of secondary structure motifs of peptide
1 estimated by the SELCON program.
11
This journal is © The Royal Society of Chemistry 2002 2244 CHEM. COMMUN. , 2002, 2244–2245
DOI: 10.1039/b206886a