Molecularly imprinted polymers (MIPs) function as synthetic
analogues
of antibody–antigen systems that provide molecular recognition.
In combination with an electrochemical interface, MIPs afford a promising
route to selectively detect a diverse range of chemical analytes and
environmental contaminants (e.g.,
per- and polyfluoroalkyl substances, PFAS). However, mechanical instabilities
and binding irreversibility may limit the practical utility as a field-deployable
sensor. Herein, we present a directed optimization of MIP-based sensors
for PFAS by varying key fabrication parameters (i.e., potential window, scan rate, molar ratio) to
modulate the mechanical properties and sensing reversibility, as measured
by atomic force microscopy (AFM)-based nanoindentation and electrochemical
methods. We demonstrate that the elastic recovery of MIP films strongly
depends on the synthesis scan rate during anodic electrochemical polymerization.
Furthermore, the increase in the elastic recovery significantly improves
the sensing reversibility and mitigates signal drift. We anticipate
that understanding the synthesis parameters and mechanical properties
of MIPs will provide insights into the development of robust and reliable
sensors for environmental monitoring.