Abstract

Self-powered immunosensors (SPIs) based on enzymatic biofuel cell (EBFC) have low sensitivity and poor stability due to the high impedance of the immune sandwich and the vulnerability of enzymes to environmental factors. Here, we applied the Faraday cage-type sensing mode on a hybrid biofuel cell (HBFC)-based SPI for the first time, which exhibited high sensitivity and stability. Cytokeratin 19 fragment (CYFRA 21-1) was used as a model analyte. Au nanoparticle-reduced graphene oxide (Au-rGO) composite was used as the supporting matrix for immunoprobe immobilized with detection antibody and glucose dehydrogenase (GDH), also the builder for Faraday cage structure on the bioanode in the presence of antigen. After the combination of immunoprobe, antigen, and the antibody on the bioanode, the Faraday cage was constructed in case the AuNP-rGO was applied as a conductive cage for electron transfer from GDH to the bioanode without passing through the poorly conductive protein. With the assistance of the Faraday cage structure, the impedance of the bioanode decreased significantly from 4000 to 300 Ω, representing a decline of over 90%. The sensitivity of the SPI, defined as the changes of open circuit voltage (OCV) per unit concentration of the CYFRA 21-1, was 68 mV [log (ng mL-1)]-1. In addition, Fe-N-C was used as an inorganic cathode material to replace enzyme for oxygen reduction reaction (ORR), which endowed the sensor with 4-week long-term stability. This work demonstrates a novel sensing platform with high sensitivity and stability, bringing the concept of hybrid biofuel cell-based self-powered sensor.

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