Metal-free, cost-efficient, redox-active electrode materials,
combining
graphene derivatives with nitrogen-rich polymelamine (PM), are widely
explored as an interface layer for electrocatalysis and an electrochemical
sensor platform. However, conventional chemical routes often yield
derivatives of PM suffering from impaired redox behavior, restricting
their electron-transfer kinetics. Herein, an optimal potentiodynamic
method has been established to electrodeposit PM on electrochemically
reduced graphene oxide (ErGO). A supporting electrolyte, containing
Cl–, enhances the formation of intermediates NH3
+ and NH2
+ at the
monomeric melamine, eventually interacting with the residual oxygenated
functional groups of ErGO to form PM. In situ Raman
spectrum analysis revealed the influence of the defective area and
the graphitization ratio on the ErGO surface during the course of
electropolymerization of melamine. Under optimal electrodeposition
conditions (E = 0–1.6 V; ν = 0.1 V/s),
the amount of electrodeposited PM on the ErGO surface was determined
to be 16.5 μg/(cycle·cm2), using electrochemical
quartz crystal microbalance analysis. An ErGO-PM-modified glassy carbon
electrode (GCE) and a screen-printed electrode exhibit the direct
electrooxidation of acyclovir (ACV). Amperometric analyses of ErGO-PM-modified
electrodes exhibited the lowest detection limit of 137.4 pM with analytical
robustness, rapid steady state, and reproducibility promising for
ACV detection in complex biological matrices.