A novel in situ-generated nanogold plasmon-enhanced photoelectrochemical aptasensor for Hg(2+) ions was fabricated using a perylene-3,4,9,10-tetracarboxylic acid/graphene (PTCA-GR) heterojunction. The fabricated photoelectrochemical aptasensor was based on thymine-Hg(2+)-thymine coordination chemistry and the plasmonic near-field absorption enhancement effect of the subsequent specific catalytic formation of nanogold. The energetic electrons from the surface plasmons of the nanogold were injected into the LUMO orbit of the organic PTCA semiconductor and then rapidly transferred to the electrode through GR due to the possible Hg(2+)-DNA molecular wires following irradiation with the visible light (λ > 450 nm) and at a bias voltage of 0.2 V. The fabricated aptasensor was linear in its response to the concentration of Hg(2+) ions in the range of 5-500 pmol L(-1), with a detection limit of 2 pmol L(-1). The presence of up to 200-fold greater concentrations of other common metal ions did not interfere with the detection of Hg(2+) ions in an aqueous system, and the results corresponded well with those obtained by ICP-MS. This novel plasmon-enhanced photoelectrochemical aptasensor exhibited good performance with its high sensitivity, good selectivity, low cost, and portable features. The strategy of the localized surface plasmon resonance through the in situ generation of noble metal nanoparticles paves the way for improvements in PEC aptasensor performance.
An innovative photoelectrochemical (PEC) biosensor platform was designed based on the in situ generation of CdS quantum dots (QDs) on graphene oxide (GO) using an enzymatic reaction. Horseradish peroxidase catalyzed the reduction of sodium thiosulfate with hydrogen peroxide to generate H2S, which reacted with Cd(2+) to form CdS QDs. CdS QDs could be photoexcited to generate an elevated photocurrent as a readout signal. This strategy offered a "green" alternative to inconvenient presynthesis procedures for the fabrication of semiconducting nanoparticles. The nanomaterials and assembly procedures were characterized by microscopy and spectroscopy techniques. Combined with immune recognition and on the basis of the PEC activity of CdS QDs on GO, the strategy was successfully applied to a PEC assay to detect carcinoembryonic antigen and displayed a wide linear range from 2.5 ng mL(-1) to 50 μg mL(-1) and a detection limit of 0.72 ng mL(-1) at a signal-to-noise ratio of 3. The PEC biosensor showed satisfactory performance for clinical sample detection and was convenient for determining high concentrations of solute without dilution. This effort offers a new opportunity for the development of numerous rapid and convenient analytical techniques using the PEC method that may be applied in the design and preparation of various solar-energy-driven applications.
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