Here, we present
a covalent nanolayer system that consists
of a
conductive and biorepulsive base layer topped by a layer carrying
biorecognition sites. The layers are built up by electropolymerization
of pyrrole derivatives that either carry polyglycerol brushes (for
biorepulsivity) or glycoside moieties (as biorecognition sites). The
polypyrrole backbone makes the resulting nanolayer systems conductive,
opening the opportunity for constructing an electrochemistry-based
sensor system. The basic concept of the sensor exploits the highly
selective binding of carbohydrates by certain harmful bacteria, as
bacterial adhesion and infection are a major threat to human health,
and thus, a sensitive and selective detection of the respective bacteria
by portable devices is highly desirable. To demonstrate the selectivity,
two strains of Escherichia coli were
selected. The first strain carries type 1 fimbriae, terminated by
a lectin called FimH, which recognizes α-d-mannopyranosides,
which is a carbohydrate that is commonly found on endothelial cells.
The otherE. coli strain was of a strain
that lacked this particular lectin. It could be demonstrated that
hybrid nanolayer systems containing a very thin carbohydrate top layer
(2 nm) show the highest discrimination (factor 80) between the different
strains. Using electrochemical impedance spectroscopy, it was possible
to quantify in vivo the type 1-fimbriated E. coli down to an optical density of OD600 = 0.0004 with a theoretical limit of 0.00005. Surprisingly, the
selectivity and sensitivity of the sensing remained the same even
in the presence of a large excess of nonbinding bacteria, making the
system useful for the rapid and selective detection of pathogens in
complex matrices. As the presented covalent nanolayer system is modularly
built, it opens the opportunity to develop a broad band of mobile
sensing devices suitable for various field applications such as bedside
diagnostics or monitoring for bacterial contamination, e.g., in bioreactors.