Currently, developing versatile, easy-to-operate, and effective signal amplification strategies hold great promise in photoelectrochemical (PEC) biosensing. Herein, an ultrasensitive polyvinylpyrrolidone-treated In 2 S 3 /WO 3 (In 2 S 3 -P/WO 3 )-functionalized paper-based PEC sensor was established for sensing ochratoxin A (OTA) based on a target-driven self-feedback (TDSF) mechanism enabled by a dual cycling tactic of PEC chemical−chemical (PECCC) redox and exonuclease III (Exo III)-assisted complementary DNA. The In 2 S 3 -P/WO 3 heterojunction structure with 3D open-structure and regulable topology was initially in situ grown on Au nanoparticlefunctionalized cellulose paper, which was served as a universal signal transducer to directly record photocurrent signals without complicated electrode modification, endowing the paper chip with admirable anti-interference ability and unexceptionable photoelectric conversion efficiency. With the assistance of Exo III-assisted cycling process, a trace amount of OTA could trigger substantial signal reporter ascorbic acid (AA) generated by the enzymatic catalysis of alkaline phosphatase, which could effectively provoke the PECCC redox cycling among the tris(2-carboxyethyl)phosphine acid, AA, and ferrocenecarboxylic at the In 2 S 3 -P/WO 3 photoelectrode, initiating TDSF signal amplification. Based on the TDSF process induced by the Exo III-assisted recycling and PECCC redox cycling strategy, the developed paper-based PEC biosensor realized ultrasensitive determination of OTA with persuasive selectivity, high stability, and excellent reproducibility. It is believed that the proposed paper-based PEC sensing platform exhibited enormous potential for the detection of other targets in bioanalysis and clinical diagnosis.

In vitro biosensing chips are urgently needed for early-stage diagnosis and real-time surveillance of epidemic diseases. Herein, a versatile zone with photothermal effects is implanted in the miniature space of a collapsible lab-on-paper photoelectrochemical biosensor for on-site detection of microRNA-141 in body fluids, which can flexibly interconnect the traditional photocurrent signal with functional temperature response. The visualized thermoresponsive results are enhanced by the exciton energy conversion between Fe3O4 nanoparticles (Fe3O4 NPs) and formed Prussian blue nanoparticles under near-infrared irradiation, which not only presents heat energy gradient variations but also generates color changes. Significantly, the controlled release of Fe3O4 NPs is actuated by a target-triggered enzyme assist strand displacement cycle strategy to efficiently improve the accuracy of target temperature signal prediction, which can concurrently mediate photoelectric signal attenuation via promoting the rapid recombination of photoexcited charge carriers on the CuInS2/CoIn2S4 electrode surface, affording dependable ultrasensitive detection results. Benefitting from the ingenious design of the versatile thermoresponsive-photoelectric sensing platform, the preliminary screening and ultrasensitive quantitative analysis can be simultaneously achieved in a single-drop sample. As a consequence, speedy prediction results and satisfied monitoring data are acquired in the ranges of 0.5 pM to 2 nM and 0.001 pM to 5 nM by measuring the temperature change and photocurrent intensity. By right of these advantages, such research paves a prospective paradigm for the manufacture of a visual, rapid, broad-spectrum, and reliable real-time surveillance platform, which allows it to be a promising candidate for epidemic disease home diagnosis and intelligent diagnosis.

Herein, a newly designed two-in-one tetrahedral DNA (TDN) nanostructure with an antifouling surface and backbone-rigidified interfacial tracks was developed for highly sensitive and selective detection of miRNA-182-5p. The well-regulated TDN tracks were assembled onto the surface of the TiO 2 /MIL-125-NH 2 -functionalized paper electrode, which efficiently avoided the obstacle of DNA strand tangling and decreased the probability of suspension during the walking process, thus greatly promoting the moving efficiency of DNA walkers. More interestingly, the TDN-modified sensing interfaces demonstrated incomparable antifouling ability against protein samples and interfering miRNAs due to the strong hydrophilic capacity and special molecular conformations, which addressed the dilemma of low sensitivity from traditional antifouling coating strategies. As a proof of concept, the designed bifunctional tetrahedron-modified paper-based photoelectrochemical sensor was successfully used to quantify miRNA-182-5p with a low detection limit of 0.09 fM and high specificity and was validated for monitoring of miRNA-182-5p in real samples. This TDN-engineered biointerface could be used as a universal platform for tracking various targets by substituting the biorecognition events, providing great promise for bioanalysis and clinical diagnosis.

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