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Rational utilization of the rich light‐bio‐matter interplay taking place in single‐cell analysis represents a new technological direction in the field. The light‐fueled operation is expected to achieve advanced photoelectrochemical (PEC) single‐cell analysis with unknown possibilities. Here, a PEC nanoreactor capable of single‐cell sampling and near zero‐background Faradaic detection of intracellular microRNA (miR) is devised by the construction of a small reaction chamber accommodating the target‐triggered hybridization chain reaction for binding the metallointercalator of [Ru(bpy)2(dppz)]2+ as the signal reporter. Light stimulation of the dsDNA/metallointercalator adduct will induce the generation of photocurrents, underpinning a zero‐biased and near zero‐background PEC method toward Faradaic detection of non‐electrogenic miR at the single‐cell level. Using this nanotool, lower miR concentration in the near‐nucleus region than that in the main cytosol was revealed. [ABSTRACT FROM AUTHOR]

Photoelectrochemical (PEC) cytosensors, a combination of the PEC process and the living‐cell assay, have emerged as a powerful tool in the analytical and biological science. This mini review provides a brief introduction of this arena and summaries the key steps about the development of PEC cytosensors with representative examples, followed by future prospects based on our own opinions. [ABSTRACT FROM AUTHOR]

Photonic (bio)electronic circuits and devices have been an enduring goal in modern photonics and electronics. Organic photoelectrochemical transistor (OPECT) interfacing light with biological world creates a substantial opportunity to this end due to the immense light−bio−matter interplay. Through modulating the invisible ionic circuit of organic electrochemical transistor (OECT) with a bipolar electrode (BPE) accommodating different semiconductor combinations, the unique photonic electronics toward logic and sensor applications are realized. Six combinations of BPEs are produced by the representative n‐type CdS/TiO2 and p‐type BiOI/NiO semiconductors, and the corresponding photonic characteristics and operation rationale are systematically investigated and explained. Designation of opto‐logic circuits and feasibility as a sensory platform are subsequently demonstrated. This work not only represents new photonic bioelectronics but also provides a generic mechanism for the design and development of advanced opto‐logics and bio‐analytics. [ABSTRACT FROM AUTHOR]

With reduced background and high sensitivity, photoelectrochemistry (PEC) may be applied as an intracellular nanotool and open a new technological direction of single‐cell study. Nevertheless, the present palette of single‐cell tools lacks such a PEC‐oriented solution. Here a dual‐functional photocathodic single‐cell nanotool capable of direct electroosmotic intracellular drug delivery and evaluation of oxidative stress is devised by engineering a target‐specific organic molecule/NiO/Ni film at the tip of a nanopipette. Specifically, the organic molecule probe serves simultaneously as the biorecognition element and sensitizer to synergize with p‐type NiO. Upon intracellular delivery at picoliter level, the oxidative stress effect will cause structural change of the organic probe, switching its optical absorption and altering the cathodic response. This work has revealed the potential of PEC single‐cell nanotool and extended the boundary of current single‐cell electroanalysis. [ABSTRACT FROM AUTHOR]

Depending on the situation, metal ions may either play beneficial roles or be harmful to human health and ecosystems. Sensitive and accurate detection of metal ions is thus a critical issue in the field of analytical sciences and great efforts have been devoted to the development of various metal ion sensors. Photoelectrochemical (PEC) detection is an emerging technique for the bio/chemical detection of metal ions, and features a fast response, low cost and high sensitivity. Using representative examples, this review will first introduce the fundamentals and summarize recent progress in the PEC detection of metal ions. In addition, interesting strategies for the design of particular PEC metal ion sensors are discussed. Challenges and opportunities in this field are also presented. [ABSTRACT FROM AUTHOR]

Using single stranded DNA (ssDNA) as a distance controller and Au nanoparticles (NPs) functionalized with ssDNA as novel energy-transfer nanoprobes, an ultrasensitive energy-transfer based photoelectrochemical protein biosensor was realized. [ABSTRACT FROM AUTHOR]

Based on the assay of DNA binding proteins upon visible light irradiation, a photoelectrochemical sensor was constructed for successfully probing a DNA–protein interaction for the first time. [ABSTRACT FROM AUTHOR]

The evolution of photoelectrochemical (PEC) bioanalysis has resulted in substantial progress in its analytical performance and biodetection applications. The aim of this review is to provide a panoramic snapshot of the state of the art in this dynamically developing field, with special emphasis on PEC DNA analysis, immunoassay, enzymatic biosensing and cell-related detection. The future prospects in this area are also evaluated and discussed. This work will serve as a useful source to inform the interested audience of the latest developments and applications in the field of PEC bioanalysis. [ABSTRACT FROM AUTHOR]

Transconductance (gm) is one important figure of merit for benchmarking organic electrochemical transistor (OECT) biosensors, which nevertheless experiences undesired fluctuation instead of keep constant during the target detection of varied concentrations. Light‐matter interplay is recently shown as a potential way to regulate the OECT characteristics, e.g. maximum gm at zero gate bias is achieved. In this work, the challenge of unstable gm is addressed by using a unique metal‐organic framework (MOF)‐derived hollow tube indium sulfide (m‐In2S3) as the photogate. Interestingly, the light irradiation on m‐In2S3 generate a straight transfer curve, leading to a stable gm that is desirable for biological application. Exemplifying by an aptasening, such a device is then tested for protein quantification with a stable sensitivity during the detection. This work features the feasibility of light‐matter interplay to achieve a stable gm in organic electronics. [ABSTRACT FROM AUTHOR]

This work is the first report on the energy transfer between CdS quantum dots and Au nanoparticles for photoelectrochemical biosensing applications. [ABSTRACT FROM AUTHOR]

Enzymatic biosensors have been valuable bioanalytical devices for analysis of diverse targets in disease diagnosis, biological and biomedical research, etc. Photoelectrochemical (PEC) bioanalysis is a recently emerged method that promptly becoming a subject of new research interests due to its attractive potential for future bioanalysis with high sensitivity and specificity. PEC enzymatic biosensors integrate the inherent sensitivities of PEC bioanalysis and the selectivity of enzymes and thus share their both advantages. Currently, PEC enzymatic biosensors have become a hot topic of significant research and the recent impetus has grown rapidly as demonstrated by increased research papers. Given the pace of advances in this area, this review will make a thorough discussion and survey on the fundamentals, sensing strategies, applications and the state of the art in PEC enzymatic biosensors, followed by future prospects based on our own opinions. We hope this work could provide an accessible introduction to PEC enzymatic biosensors for any scientist. [ABSTRACT FROM AUTHOR]

Photoelectrochemical (PEC) bioanalysis represents a unique and dynamically developing methodology that offers an elegant route for sensitive biomolecular detection. Aptamers are synthetic nucleic acid molecules whose binding characteristics can rival those of protein antibodies. Originated from the fusion of PEC bioanalysis and aptamers, PEC aptasensing has rapidly becoming a subject of new research interests in recent years. Using illustrative examples, this review provides the introductory concept, bioanalysis development, signaling strategies, and the state of the art in this field. The future prospects are also discussed. [ABSTRACT FROM AUTHOR]

Abstract: A novel photoelectrochemical immunosensor based on TiO2/CdS hybrid modified electrode was developed. The TiO2/CdS hybrid modified electrode was obtained by alternately dipping the TiO2 modified indium–tin oxide (ITO) electrode into the [Cd(NH3)4]2+ and S2− solution repeatedly. Compared with the routine method using Cd2+ solution for CdS deposition, the as obtained TiO2/CdS electrode showed enhanced photocurrent intensity with fewer coating times. After the ITO/TiO2/CdS electrode was coated with chitosan (CS), α-fetoprotein (AFP) antibodies were covalently conjugated on the surface of the electrode. Thus, a label-free photoelectrochemical immunosensor for the detection of AFP was developed by monitoring the changes in the photocurrent signals of the electrode resulting from the immunoreaction. The immunosensor displayed a linear response to AFP in the ranges from 50pg/mL to 50ng/mL with a relatively low detection limit of 40pg/ml. The photoelectrochemical results for the detection of AFP in five human sera showed acceptable accuracy. The method is simple, sensitive and specific. Moreover, the studied immunosensor possessed acceptable reproducibility and storage stability. The proposed methodology was potentially attractive for clinical immunoassay. [Copyright &y& Elsevier]

Abstract: Dopamine-coordinated photoactive TiO2 nanoporous films with a wide excitation range of light in the visible region (up to 580nm) were prepared and used for sensitive detection of NADH. Colloidal TiO2 was firstly covered on an indium–tin oxide (ITO) electrode surface and sintered at 450°C to form a nanoporous TiO2 film, then the electrode was dipped in a dopamine solution to form a dopamine–TiO2 charge transfer complex via coordinating dopamine with undercoordinated titanium atoms on the electrode surface. This charge transfer complex provided an anodic photocurrent under visible light and the photocurrent could be largely enhanced by NADH. The photocurrent enhancement might be due to the electron transfer between NADH and the holes localized on dopamine. A new photoelectrochemical methodology for sensitive detection of NADH at a relatively low potential was developed. The detection limit of NADH was 1.4×10−7 M, and the detection range could extend up to 1.2×10−4 M. The dopamine–TiO2 modified electrode exhibits its major advantages such as effective electronic transducer, fast response and easy fabrication for photoelectrochemical determination of NADH. This strategy largely reduces the destructive effect of UV light and the photogenerated holes of illuminated TiO2 to biomolecules and opens a new avenue for the applications of TiO2 in photoelectrochemical biosensing. [Copyright &y& Elsevier]

We report herein the energy transfer (ET) between semiconducting polymer dots (Pdots) and gold nanoparticles (Au NPs) in a photoelectrochemical (PEC) system and its feasibility for cathodic bioanalysis application. Specifically, COOH-capped Pdots were first fabricated and then assembled onto the indium-tin oxide (ITO) surface, followed by the modification of single-strand (ss) DNA probe (pDNA). After the DNA hybridization with the Au NPtethered complementary ssDNA (Au NP-tDNA), the Au NPs were brought into the close proximity of Pdots. Upon light stimulation, photoluminescence (PL) was annihilated, fluorescence was attenuated, and the photocurrent intensity was evidently decreased. This ET-based PEC DNA sensor exhibited a linear range from 1 fM to 10 pM with a detection limit of 0.97 fM at a signal-to-noise ratio of 3. The present work first exploited the ET between Pdots and Au NPs, and we believe this phenomenon will spark new interest in the study of various Pdots-based ET-influenced PEC systems and thus catalyze increasing studies for specific bioanalytical purposes. [ABSTRACT FROM AUTHOR]

Photoelectrochemical (PEC) bioanalysis is a newly developed methodology that provides an exquisite route for innovative biomolecular detection. Quantum dots (QDs) are semiconductor nanocrystals with unique photophysical properties that have attracted tremendous attentions among the analytical community. QDs-based PEC bioanalysis comprises an important research hotspot in the field of PEC bioanalysis due to its combined advantages and potentials. Currently, it has ignited increasing interests as demonstrated by increased research papers. This review aims to cover the most recent advances in this field. With the discussion of recent examples of QDs-PEC bioanalysis from the literatures, special emphasis will be placed on work reporting on fundamental advances in the signaling strategies of QDs-based PEC bioanalysis from 2013 to now. Future prospects in this field are also discussed. [ABSTRACT FROM AUTHOR]

This work reports the use of compositionally heterogeneous asymmetric Ag@Au core–satellite nanoassembly functionalized with DNA sequence as unique signaling nanoprobes for the realization of new energy-transfer-based photoelectrochemical (PEC) immunoassay of prostate- specific antigen (PSA). Specifically, the Ag@Au asymmetric core–satellite nanoassemblies (Ag@Au ACS) were fabricated on a two-dimensional glass substrate by a modified controlled assembly technique, and then functionalized with DNA sequences containing PSA aptamers as signaling nanoprobes. Then, the sandwich complexing between the PSA, its antibodies, and the signaling nanoprobes was performed on a CdS QDs modified indium tin oxide (ITO) electrode. The single stranded DNA can server as a facile mediator that place the Ag@Au ACS in proximity of CdS QDs, stimulating the interparticle exciton–plasmon interactions between Ag@Au ACS and CdS QDs and thus quenching the excitonic states in the latter. Since the damping effect is closely related to the target concentration, a novel energy-transfer-based PEC bioanalysis could be achieved for the sensitive and specific PSA assay. The developed biosensor displayed a linear range from 1.0×10 −11 g mL −1 to 1.0×10 −7 g mL −1 and the detection limit was experimentally found to be of 0.3×10 –13 g mL −1 . This strategy used the Ag@Au ACS-DNA signaling nanoprobes and overcame the deficiency of short operating distance of the energy transfer process for feasible PEC immunoassay. More significantly, it provided a way to couple the plasmonic properties of the Ag NPs and Au NPs in a single PEC bioanalytical system. We expected this work could inspire more interests and further investigations on the advanced engineering of the core–satellite or other judiciously designed nanostructures for new PEC bioanalytical uses with novel properties. [ABSTRACT FROM AUTHOR]

Herein, on the basis of the alkaline phosphate (ALP) induced reaction, a simultaneous photoelectrochemical (PEC) and visualized immunoassay has been established for the detection of β-human chorionic gonadotrophin (β-HCG). Specifically, in the proposed system, ALP stimulated the oxidative hydrolyzing transformation of 5-bromo-4-chloro-3-indoyl phosphate (BCIP) to an indigo precipitation, generating an insulating layer that impeded the interfacial mass and electron transfer and thus the photocurrent production. Meanwhile, a visualized detection could be performed according to the change of color intensity. Upon proper experimental conditions, the protocol possessed a detection range of 0.5–1000 IU/L with a detection limit of (0.20±0.011) IU/L toward β-HCG. With high sensitivity and specificity, this work presents the first general protocol for simultaneous PEC and visualized detection, which could be easily extended to addressing numerous other targets. [ABSTRACT FROM AUTHOR]

Herein the influence of ultrasmall Ag nanoclusters (Ag NCs) against CdS quantum dots (QDs) in a photoelectrochemical (PEC) nanosystem was exploited for the first time, based on which a novel PEC bioanalysis was successfully developed via the efficient quenching effect of Ag NCs against the CdS QDs. In a model system, DNA assay was achieved by using molecular beacon (MB) probes anchored on a CdS QDs modified electrode, and the MB probes contain two segments that can hybridize with both target DNA sequence and the label of DNA encapsulated Ag NCs. After the MB probe was unfolded by the target DNA sequence, the labels of oligonucleotide encapsulated Ag NCs would be brought in close proximity to the CdS QDs electrode surface, and efficient photocurrent quenching of QDs could be resulted from an energy transfer process that originated from NCs. Thus, by monitoring the attenuation in the photocurrent signal, an elegant and sensitive PEC DNA bioanalysis could be accomplished. The developed biosensor displayed a linear range from 1.0 pM to 10 nM and the detection limit was experimentally found to be of 0.3 pM. This work presents a feasible signaling principle that could act as a common basis for general PEC bioanalysis development. [ABSTRACT FROM AUTHOR]

A novel photoelectrochemical (PEC) sensor for mercury ions (Hg 2 + ) was fabricated based on the energy transfer (ET) between CdS quantum dots (QDs) and Au nanoparticles (NPs) with the formation of T–Hg 2 + –T pairs. In the presence of Hg 2 + ions, a T-rich single-strand (ss) DNA labeled with Au NPs could hybridize with another T-rich ssDNA anchored on the CdS QDs modified electrode, through T–Hg 2 + –T interactions, rendering the Au NPs in close proximity with the CdS QDs and hence the photocurrent decrease due to the ET between the CdS QDs and the Au NPs. Under the optimal condition, the photocurrent decrease was proportional to the Hg 2 + concentration, ranging from 3.0 × 10 − 9 to 1.0 × 10 − 7 M, with the detection limit of 6.0 × 10 − 10 M. [ABSTRACT FROM AUTHOR]

Abstract: Photoelectrochemical (PEC) bioanalysis has attracted considerable research interest due to its desirable properties, and its rapid evolution has resulted in great progress in bioanalytical applications. This mini review aims to provide a snapshot of the introductory concepts and main principles of PEC bioanalysis, as well as the basic classification of the established signaling strategies with recent illustrative examples. [Copyright &y& Elsevier]

Abstract: A sensitive photoelectrochemical (PEC) approach for Pb2+ sensing was achieved firstly with the coupling of G-quadruplex-based DNAzyme and biocatalytic precipitation (BCP) on a CdS quantum dots electrode. Pb2+ can induce the conformational change of K+-stabilized G-quadruplex-based DNAzyme, leading to the decrease of the catalytic activity to H2O2-mediated 4-chloro-1-naphthol oxidation (BCP reaction). From the respective BCP reaction that monitors the event of DNAzyme deactivation, a novel PEC Pb2+ sensor could be realized with a detection limit of 1.0×10−8 M. [Copyright &y& Elsevier]

Abstract: We demonstrated herein a newly developed photoelectrochemical cell-sensor for the determination of SMMC-7721 human hepatoma carcinoma cells (SMMC-7721 cells) by using a photosensitive CdS-polyamidoamine (G4) nano-composite film (CdS-PAMAM). The film was generated by electrodeposition method. The presence of PAMAM in the film eliminated the surface defects of CdS nanoparticles and therefore resulted in a greatly enhanced photocurrent and a reduced dark current. In the presence of the electron donor ascorbic acid (AA), the photoexcitation of this modified electrode potentiostated at 0V versus Ag/AgCl led to an anodic photocurrent. As a result of the covalent coupling reactions, a layer of concanavalin A (ConA) was firmly bound to the functionalized CdS-PAMAM film via glutaraldehyde bridges. The resulting modified electrodes were tested as sensors for SMMC-7721 cell capture and detection via affinity interactions between ConA and mannosyl groups on cell surface. The cell concentration was measured from 5.0×103 to 1.0×107 cellsmL−1 through the decrease in photocurrent intensity resulting from its specific binding onto the photosensitive film, the detection limit being 5.0×103 cellsmL−1. [Copyright &y& Elsevier]

Abstract: The coupling of biocatalytic precipitation (BCP) to photoelectrochemical (PEC) biosensing for the development of rapid PEC sensors with ultrahigh sensitivity and excellent anti-interference ability is successfully realized. Horseradish peroxidase (HRP) was immobilized on the matrix of TiO2/CdS and 4-chloro-1-naphthol (4-CN) was chosen for the BCP-amplified PEC detection of H2O2. The HRP accelerated oxidation of 4-CN by H2O2 would yield insoluble product on the photoelectrode surface, on the basis of which the photocurrent be influenced. The detection limit of 5.0×10−10 M (S/N=3) for the determination of H2O2 was achieved. [Copyright &y& Elsevier]