Photoelectrochemical (PEC) sensors are relatively new sensing platforms with high detection sensitivity and low cost. However, the current PEC biosensors dependent on ultraviolet or visible light as the exciting resource cause injuries to biological samples and systems, which restrains the applications in complicated matrixes. Herein, a near-infrared light (NIR)-initiated PEC biosensor based on NaYF 4 :Yb,Tm@NaYF 4 @ TiO 2 @CdS (csUCNRs@TiO 2 @CdS) was constructed for sensitive detection of acute myocardial infarction (AMI)-related miRNA-133a in an immobilization-free format coupled with a hybridization chain reaction and a redox circle signal amplification strategy. A low-energy 980 nm NIR incident laser was converted to 300−480 nm light to excite the adjacent TiO 2 @CdS photosensitive shell to generate photocurrent by NaYF 4 :Yb,Tm@NaYF 4 upconversion nanorods. Also, magnetic beads were employed for the homogeneous determination of target miRNA-133a to reduce the recognition steric hindrance and improve the detection sensitivity. The photocurrent response was positively correlated with the level of ascorbic acid as the energy donor to consume photoacoustic holes produced on the surface of csUCNRs@TiO 2 @CdS, which was generated by alkaline phosphatase catalyzation and regenerated by tris(2-carboxyethyl) phosphine reduction upon the appearance of miRNA-133a. Exerting a NIR-light-driven and immobilization-free strategy, the asconstructed biosensor displayed linearly sensitive and selective determination of miRNA-133a with a detection limit of 36.12 aM. More significantly, the assay method provided a new concept of the PEC sensing strategy driven by NIR light to detect diverse biomarkers with pronounced sensitivity, light stability, and low photodamage.

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A novel photoelectrochemical (PEC) aptasensor was fabricated for DNA detection based on the coupling of cosensitization and peroxidase-like catalytic activity. Specifically, the surfaces of branched-TiO 2 nanorods (B-TiO 2 NRs) were modified with Cd 2+ and S 2+ to obtain B-TiO 2 NRs/CdS hybrid structures, which were subsequently used as matrices to immobilize hairpin DNA (hDNA) probes. CdTe/TCPP (TCPP = meso-tetra(4-carboxyphenyl)-porphine) used for signal amplification was labeled on the terminal of the hDNA probe. Without the target DNA (tDNA) presence, the immobilized hDNA probe with CdTe/TCPP possessed a hairpin form and was located near the B-TiO 2 NRs/CdS electrode surface, forming a cosensitized structure formation and then generating strong photocurrent with H 2 O 2 as the electron donor. During detection, the specific recognition of tDNA by the sensing hDNA probe triggered the formation of the G-quadruplex/hemin DNAzyme, which effectively catalyzed the decomposition of H 2 O 2 . Meanwhile, cosensitization disappeared when the hDNA probe hybridized with tDNA, further reducing the photocurrent. With a double-signal amplification strategy, the sensing platform designed in this work demonstrated a linear detection ability in the 0.5 fM−5 nM range with a detection limit equal to 0.14 fM. Notably, through encoding in the base sequences of the hDNA and marking it, a versatile PEC platform could be structured for the detection of various DNA targets, which could promise applications in point-of-care diagnostic fields.

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