An inorganic-framework molecularly imprinted NiAl layered
double
hydroxide (MI-NiAl-LDH) with specific template molecule (glyphosate
pesticide, Glyp) recognition ability was prepared on Ni nanorod arrays
(Ni NRAs) through electrodeposition followed by a low-temperature
O2 plasma treatment. The freestanding Ni/MI-NiAl-LDH NRA
electrode had highly enhanced sensitivity and selectivity. The electrocatalytic
oxidation of Glyp was proposed to occur at Ni3+ centers
in MI-NiAl-LDH, and the current response depended linearly on the
Glyp concentration from 10.0 nmol/L to 1.0 μmol/L (R
2 = 0.9906), with the limit of detection (LOD) being 3.1
nmol/L (S/N = 3). An exceptional discriminating capability with tolerance
for other similar organophosphorus compounds was achieved. Molecular
imprinting (N and P residues) affected the electronic structure of
NiAl-LDH, triggering the formation of highly active NiOOH sites at
relatively lower anodic potentials and substantially enhancing the
electrocatalytic oxidation ability of the NiAl-LDH interface toward
the C–N bonds in Glyp. In combination with the surface enrichment
effect of MI-NiAl-LDH toward template molecules, the electrochemical
oxidation signal intensity of Glyp increased significantly, with a
greater peak separation from interfering molecules. These results
challenge the common belief that the excellent performance of inorganic-framework
molecularly imprinted interfaces arises from their specific adsorption
of template molecules, providing new insight into the development
of high-performance organic-pollutant-sensing electrodes.
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