Redox-Reactive Field-Effect Transistor Nanodevices for the Direct Monitoring of Small Metabolites in Biofluids toward Implantable Nanosensors Arrays

摘要

Chemically modified field-effect transistor (FET) nanodevices were shown to be a selective and extremely sensitive detection platform. In FET-based sensors, signal amplification and transduction is based on electrostatic gating of the nanometric semiconductor channel by analyte-receptor interactions, which measurably affect the transconductance of the device. However, chemically modified FETs must overcome several fundamental limitations before they can be effectively deployed as real-time sensors for bioevents occurring on their surface in complex biofluids. Here, we demonstrate the development of amperoFET devices for the real-time continuous monitoring of small molecular metabolites in biofluids. The surface of the nanowires is covalently modified with a redox reversible moiety, which is easily oxidized in the presence of H2O2. The reversible redox transformation of the surfaceconfined molecules is carried out by a hot electron injection mechanism, conducted simply by the modulation of the source- drain current through the nanoFET sensing device. By this approach, electrons may be injected by the nanowire element into the surface-confined redox moiety and thus maintain a whole-electrically actuated redox system in which the oxidation state is completely controlled by the current applied to the amperoFET system. The modulation of the source-drain current allows the control of the reduced versus oxidized redox moieties population on the nanowire surface, and this, in turn, is applied as the main sensing mechanism. At a given constant source-drain and gate voltage, the chemical perturbation exerted by the presence of chemical oxidants in the tested biofluid will lead to a measurable conductance change. Alteration in the concentration of the specific metabolite will chemically regulate the extent of perturbation applied to the redox system, which can be utilized for the quantification of the molecular metabolite of interest. These 'equilibrium' -type sensors are fully electrically operated and can be further used in implantable sensing applications.