Herein,
fluorescent gold nanoclusters (AuNCs) and horseradish peroxidase
(HRP) were simultaneously embedded into self-assembled dipeptide supramolecular
films of N-fluorenylmethoxycarbonyl diphenylalanine
(Fmoc-FF) on the surface of ITO electrodes (Fmoc-FF/AuNCs/HRP) by
using a simple single-step process. In the films, both the fluorescence
property of AuNCs and the bioelectrocatalytic property of HRP were
well maintained and could be reversibly regulated by pH-sensitive
structural changes in the Fmoc-FF hydrogel films. Cu(II)/EDTA in the
solution could lead to the aggregation/disaggregation of AuNCs and
further quenching/dequenching the fluorescence signal from the films.
Meanwhile, the blue complexes formed by Cu(II) and EDTA could produce
a UV–vis signal in the solution. In addition, the coordinated
Cu(II) in the films enhanced the electrocatalytic capacity toward
the reduction of H2O2 and could switch the current
signal. A biomolecular logic circuit was built based on the smart
film electrode system by using pH, the concentrations of EDTA, Cu(II)
and H2O2 as inputs, while the fluorescence intensity
(FL), current (I) and UV–vis extinction (E) of the solution as outputs. Various logic devices were
fabricated using the uniform platform, consisting of an encoder/decoder,
demultiplexer, dual-transfer gate, keypad lock, digital comparator,
half adder, and controlled NOT (CNOT) gate. Specifically, an electronic
three-value logic gate, gullibility (ANY) gate, was
first mimicked in this biocomputing system. This work not only demonstrated
the construction of a new type of multivalued logic gate by using
a dipeptide micromolecular matrix but also provided a new approach
for designing sophisticated biologic functions, establishing smart
multianalyte biosensing or fabricating biology information processing
through the use of a simple film system.