Dual-mode self-powered photoelectrochemical and colorimetric determination of procalcitonin accomplished by multienzyme-expressed Ni4Cu2 bimetallic hollow nanospheres and spherical nanoflower-MoS2/Cu2ZnSnS4/Bi2S3.

Bacterial infections, viral infections and autoimmune diseases pose a considerable threat to human health. Procalcitonin (PCT) has emerged as a biomarker for the detection of these diseases. To ensure accurate and reliable results, we propose a dual-mode approach that incorporates self-validation and self-correction mechanisms. Herein, we develop a dual-mode self-powered photoelectrochemical (PEC) and colorimetric sensor to determine PCT. The self-powered PEC sensor was constructed with a photoanode of spherical nanoflower-MoS2/Cu2ZnSnS4/Bi2S3 material and a photocathode of CuInS2 material. Ni4Cu2 bimetallic hollow nanospheres (BHNs) possess superoxide dismutase and catalase performance, which facilitate superoxide anion radical (·O2-) and H2O2 circulating generation, promoting the separation of photogenerated electrons and holes to amplify photocurrent signal. Thus Ni4Cu2 BHNs is used as a marker material for PEC sensor. Meanwhile, in colorimetric mode, Ni4Cu2 BHNs converts blue oxTMB to a colourless TMB for colorimetric detection of PCT. Based on this principle, dual-mode determination of PCT with high sensitivity is achieved. The dual-mode method not only demonstrates outstanding properties and practicability, but also presents an effective, highly efficient and reliable method for detecting PCT.

A photoelectrochemical aptasensing platform assembled at the heterojunction interface of Cu3BiS3 sensitized CuV2O6 for bisphenol A.

The interaction between the sensitive interfaces of photoelectrochemical (PEC) semiconductor nanomaterials and microscopic matter creates endless potential for the efficient detection of endocrine disruptor. This work presents the development of a high-efficiency PEC aptasensor for bisphenol A (BPA) monitoring based on Cu3BiS3 sensitized CuV2O6 nanocomposites with exceptional visible-light PEC activity. We implemented the integration of Cu3BiS3 nanosheet photosensitizer to sensitize the CuV2O6 nanowire structure that was synthesized utilizing a facile hydrothermal approach. The band gap alignment between Cu3BiS3 and CuV2O6 facilitated enduring PEC response yielding an efficient interfacial structure. The surface of the CuV2O6/Cu3BiS3 electrode was modified with BPA aptamer, enabling specific binding with BPA and precise quantification of its content. The developed aptamer sensors possess a wide detection range of 5.00 × 10-1 to 5.00 × 104 ng/mL, and a low detection limit of 1.60 × 10-1 ng/mL (at S/N = 3). After undergoing 20 testing cycles and enduring long-term storage, the sensor maintained its stability and showcased excellent repeatability and reproducibility. This study presents a promising methodology for the detection of BPA in environmental settings.

A self-powered photoelectrochemical biosensing platform for H-FABP monitoring mediated by CsPbBr3@COF-V.

Advanced bioelectronic detection based on the integration of modern optical electronics and biological systems has a broad prospect. The strategy of cathode signal amplification in self-powered photoelectrochemical (PEC) immunosensors with excellent performance is rarely reported in the field of immune analysis. Herein, the work demonstrates a self-powered PEC biosensor formed with BiOI photocathode and WO3/SnS2/ZnS photoanode, and CsPbBr3@COF-V was used as the photocathode signal quenching source for the quantitative monitoring of heart fatty acid binding protein (H-FABP). The high efficiency and stable self-powered biosensor formed not only provides continuous and powerful photocurrent response for bioanalysis through reasonable stepped band structure, but also effectively eliminates the interference of reducing substances. The quenching source CsPbBr3@COF-V greatly affects the photocurrent response due to steric hindrance, weak conductivity, competition with the substrate for dissolved oxygen and excitation light source. And the intervention of this key factor achieves multiple signal amplification effect and opens up an innovative vision for self-powered PEC immunosensor. Taking H-FABP as a representative analyte, the proposed signal amplification self-powered photoelectrochemical presents a broad linear range from 0.0005 to 150 ng/mL with the detection limit of 0.19 pg/mL.

A split-type photoelectrochemical immunosensing platform based on atom-efficient cation exchange for physiological monitoring.

Ultrasensitive and accurate physiological monitoring is of great significance for disease diagnosis and treatment. In this project, an efficient photoelectrochemical (PEC) split-type sensor on the basis of controlled release strategy was established with great success. Heterojunction formation between g-C3N4 and Zn-doped CdS improved the visible light absorption efficiency, reduced carrier complexation, improved the PEC signal, and increased the stability of the PEC platform. Compared to the traditional model of immunosensors, the process of antigen-antibody specific binding was done in a 96 microplate, and the sensor separated the immune reaction from the photoelectrochemical conversion process, eliminating mutual interference. Cu2O nanocubes were used to label the second antibody (Ab2), and acid etching using HNO3 released a large amount of divalent copper ions, which exchanged cations with Cd2+ in the substrate material, causing a sharp drop in photocurrent and improving the sensitivity of the sensor. Under the optimized experimental conditions, the PEC sensor based on the controlled release strategy for CYFRA21-1 target detection had a wide concentration linear range of 5 × 10-5 to 100 ng/mL with a low detection limit of 0.0167 pg/mL (S/N = 3). This intelligent response variation pattern could also offer the possibility of additional clinical applications for other target detection.

Split-Type Photoelectrochemical/Visual Sensing Platform Based on SnO2/MgIn2S4/Zn0.1Cd0.9S Composites and Au@Fe3O4 Nanoparticles for Ultrasensitive Detection of Neuron Specific Enolase.

Herein, a novel dual mode detection system of split-type photoelectrochemical (PEC) and visual immunoassay was developed to detect neuron specific enolase (NSE), which achieved simultaneous and reliable NSE detection due to the completely different signal readouts and transduction mechanism. Specifically, specific reactions of antigens and antibodies were performed in 96-microwell plates. Gold nanoparticle (Au NP)-loaded Fe3O4 (Au@Fe3O4) NPs were used as secondary antibody markers and signal regulators, which could produce a blue-colored solution in the presence of 3,3',5,5'-tetramethylbenzidine (TMB) and H2O2 because of its peroxidase-like activity. Therefore, the visual detection of NSE was realized, making the results more intuitive. Meanwhile, the above biological process could also be used as part of the split-type PEC sensing platform. Oxidized TMB and Fe3+ were consumptive agents of the electron donor, which both realized the double quenching of PEC signal generated by the SnO2/MgIn2S4/Zn0.1Cd0.9S composites. Owing to the waterfall band structure, SnO2/MgIn2S4/Zn0.1Cd0.9S composites partially absorb visible light and effectively inhibit the electron-hole recombination, thereby providing significantly enhanced and stable initial signal. On the basis of the multiple signal amplification strategy and the split-type mode, NSE could be sensitively detected with a low detection limit of 14.0 fg·mL-1 (S/N = 3) and a wide linear range from 50.0 fg·mL-1 to 50.0 ng·mL-1.

MoSe2/CdSe Heterojunction Destruction by Cation Exchange for Photoelectrochemical Immunoassays with a Controlled-Release Strategy.

Herein, a split-type immunoassay strategy instigated by cation exchange (CE) and changing the capacity of an electron donor in an electrolyte solution is optimized, namely, for differentiating the biological-specific binding assay and photoelectrochemical (PEC) analysis. MoSe2/CdSe, a Z-scheme heterojunction with efficient visible light absorption and a low recombination of carriers, is used as a photoelectrode substrate. Silver ions (Ag+) as the initiator of CE are generated by the acidolysis of evenly loaded silver nanoparticles on mesoporous silica nanospheres (MSNs). The theoretical calculation and experimental results confirm that Ag+ replaces Cd2+ in CdSe and retains the crystal structure of MoSe2. However, this behavior destroys the perfectly matched heterojunction structure and introduces defects, which led to the reduction of the photocurrent response. In addition, ascorbate oxidase in combination with MSNs can be used as a consumptive agent of the electron donor, which further improves the sensitivity and reliability of the sensor. As a proof of principle, neuron-specific enolase was applied to elucidate the potential application of the PEC immunoassay in clinical diagnosis, and the obtained linear range of the sensor was from 0.0001 to 100 ng/mL with a detection limit of 28 fg/mL (S/N = 3).

Rationally engineered high-performance BiVO4/Ag3VO4/SnS2 photoelectrodes for ultrasensitive immunosensing of CYFRA21-1 based on HRP-tyramine-triggered insoluble precipitates.

A photoelectrochemical (PEC) biosensor capable of detecting cytokeratin 19 fragment 21-1 (CYFRA21-1) was optimized by taking advantage of the powerful conjugate repeats of horseradish peroxidase and tyramine (HRP-tyramine)-triggered enzymatic biocatalytic precipitation (BCP) on high-performance BiVO4/Ag3VO4/SnS2 photoelectrodes. Compared with the ubiquitous BCP strategy, we identified a design supporting conjugate repeats generated by HRP and tyramine-triggered immeasurable insoluble precipitates in the presence of hydrogen peroxide and 4-chloro-1-phenol (4-CN), and the steric hindrance improved sensitivity. Moreover, by virtue of BiVO4, Ag3VO4, SnS2 excellent level matching structure and chemical stability, a heterojunction (BiVO4/Ag3VO4/SnS2) with high light absorption efficiency has been successfully prepared. The novel heterostructure system of BiVO4/Ag3VO4/SnS2 with high detection current and low background signal exhibited high-performance PEC determination. Generally, the hitherto untapped biosensor resource realized the sensitive detection of CYFRA21-1 with a wide linear range from 50 fg/mL to 200 ng/mL, and a detection limit of 15 fg/mL, which illustrated the potential for biotechnological applications.

Antigen down format photoelectrochemical analysis supported by fullerene functionalized Sn3O4.

Herein, a smart competitive-type photoelectrochemical (PEC) sensor based on an antigen-down (Ag-down) format for procalcitonin (PCT) detection is proposed. A fullerene sensitized flower-like Sn3O4 nano-structure is used as the photoactive platform, and FeS2 is labeled on the secondary antibody as a signal adjusting element. The sensor exhibits excellent sensitivity and great stability.