Photoelectrochemical (PEC) DNA bioanalysis has been drawing more attention in recent years due to the advantages of PEC technique and the vital importance of DNA biomolecules. DNAzymes are unique ...catalytic nucleic acid molecules that are capable of catalyzing specific biochemical reactions. Using the target-binding-induced conformation change of hairpin DNA probe to hemin/G-quadruplex-based DNAzyme and a plasmonic Au@Ag nanoparticles (NPs)/TiO
nanorods (NRs)/fluorine-doped tin oxide (FTO) heterostructured photoelectrode, this work reported a novel and sensitive PEC DNA analysis on the basis of a DNAzyme-stimulated biocatalytic precipitation (BCP) strategy. In such a design, the BCP-induced decrease of plasmonic photocurrent can be related to the target-responsive formation of DNAzymes and thus be monitored to assay the target DNA from 0.1 and 100 nM. In brief, with a plasmonic photoelectrode and a hairpin probe, this work reported a general plasmonic DNAzyme-based PEC DNA analysis, which could also be easily extended to aptasensing toward numerous targets of interest.
Energy transfer (ET) in photoelectrochemical (PEC) bioanalysis is usually generated between noble metal nanoparticles (NPs) and traditional inorganic quantum dots (QDs). Using the innovative polymer ...dot (Pdot)-involved ET, this work reports the first signal-on and cathodic PEC bioanalysis toward telomerase (TE) activity in cell extracts. Specifically, the sequential binding of capture DNA (cDNA), telomerase primer sequence (TS), and Au NP-labeled probe DNA (Au NP-pDNA) on the electrode would place the Au NPs in close proximity of the Pdots, leading to obvious quenching of the cathodic photocurrent. The subsequent extension of the TS by TE in the presence of deoxyribonucleoside triphosphates (dNTPs) would then release the Ag NP-pDNA from the electrode, leading to the recovery of the photocurrent. On the basis of the Au NP-induced photocurrent quenching and the recovery of Pdots, a sensitive biosensor could thus be developed by tracking the photocurrents to probe the TE activity. This strategy allows for signal-on and cathodic PEC bioanalysis of TE, which can be easily extended for numerous other targets of interest. We believe this work could offer a new perspective for the rational implementation of Pdot-involved ET for advanced PEC bioanalysis.
Liposomal photoelectrochemical (PEC) bioanalysis has recently emerged and exhibited great potential in sensitive biomolecular detection. Exploration of the facile and efficient route for advanced ...liposomal PEC bioanalysis is highly appealing. In this work, we report the split-type liposomal PEC immunoassay system consisting of sandwich immunorecognition, CdS quantum dots (QDs)-loaded liposomes (QDLL), and the release and subsequent capture of the QDs by a separated TiO2 nanotubes (NTs) electrode. The system elegantly operated upon the protein binding and lysis treatment of CdS QDLL labels within the 96-well plate, and then the CdS QDs-enabled sensitization of TiO2 NTs electrode. Exemplified by cardiac markers troponin I (cTnI) as target, the proposed system achieved efficient activation of TiO2 NTs electrode and thus the signal generation toward the split-type PEC immunoassay. This work features the first use of QDs for liposomal PEC bioanalysis and is expected to inspire more interests in the design and implementation of numerous QDs-involved liposomal PEC bioanalysis.
Abstract Reproducing human visual functions with artificial devices is a long‐standing goal of the neuromorphic domain. However, emulating the chemical language communication of the visual system in ...fluids remains a grand challenge. Here, a “multi‐color” hydrogel‐based photoelectrochemical retinomorphic synapse is reported with unique chemical‐ionic‐electrical signaling in an aqueous electrolyte that enables, e.g., color perception and biomolecule‐mediated synaptic plasticity. Based on the specific enzyme‐catalyzed chromogenic reactions, three multifunctional colored hydrogels are developed, which can not only synergize with the Bi 2 S 3 photogate to recognize the primary colors but also synergize with a given polymeric channel to promote the long‐term memory of the system. A synaptic array is further constructed for sensing color images and biomolecule‐coded information communication. Taking advantage of the versatile biochemistry, the biochemical‐driven reversible photoelectric response of the cone cell is further mimicked. This work introduces rich chemical designs into retinomorphic devices, providing a perspective for replicating the human visual system in fluids.
Organic photoelectrochemical transistor (OPECT) has shown substantial potential in the development of next-generation bioanalysis yet is limited by the either-or situation between the photoelectrode ...types and the channel types. Inspired by the dual-photoelectrode systems, we propose a new architecture of dual-engine OPECT for enhanced signal modulation and its biosensing application. Exemplified by incorporating the CdS/Bi2S3 photoanode and Cu2O photocathode within the gate-source circuit of Ag/AgCl-gated poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) channel, the device shows enhanced modulation capability and larger transconductance (g m) against the single-photoelectrode ones. Moreover, the light irritation upon the device effectively shifts the peak value of g m to zero gate voltage without degradation and generates larger current steps that are advantageous for the sensitive bioanalysis. Based on the as-developed dual-photoelectrode OPECT, target-mediated recycling and etching reactions are designed upon the CdS/Bi2S3, which could result in dual signal amplification and realize the sensitive microRNA-155 biodetection with a linear range from 1 fM to 100 pM and a lower detection limit of 0.12 fM.
This Letter reports a novel synthetic methodology for the fabrication of three-dimensional (3D) nanostructured CdS@carbon fiber (CF) networks and the validation of its feasibility for applications as ...a general platform for photoelectrochemical (PEC) bioanalysis. Specifically, 3D architectures are currently attracting increasing attention in various fields due to their intriguing properties, while CdS has been most widely utilized for PEC bioanalysis applications because of its narrow band gap, proper conduction band, and stable photocurrent generation. Using CdS as a representative material, this work realized the innovative synthesis of 3D CdS@CF networks via a simple solvothermal process. Exemplified by the sandwich immunoassay of fatty-acid-binding protein (FABP), the as-fabricated 3D CdS@CF networks exhibited superior properties, and the assay demonstrated good performance in terms of sensitivity and selectivity. This work features a novel fabrication of 3D CdS@CF networks that can serve as a general platform for PEC bioanalysis. The methodology reported here is expected to inspire new interest for the fabrication of other 3D nanostructured Cd-chalcogenide (S, Se, Te)@CF networks for wide applications in biomolecular detection and beyond.
DNA intercalation has increasingly been studied for various scenario implementations due to the diverse functions of DNA/intercalators. Nascent organic photoelectrochemical transistor (OPECT) ...biosensing taking place in organic electronics and photoelectrochemical bioanalysis represents a promising technological frontier in the arena. In this work, we first devise DNA intercalation-enabled OPECT for miRNA detection with a superior gain up to 17100. Intercalation of Ru(bpy)2dppz2+ within the miRNA-initiated hybrid chain reaction (HCR)-derived duplex DNA is realized for producing anodic photocurrent upon light stimulation, causing the corresponding target-dependent alternation in gate voltage (VG) and hence the modulated channel current (IDS) of poly (3,4-ethylenedioxythiophene) doped with poly (styrene sulfonate) (PEDOT:PSS) under specific drain voltage (VDS) for quantitative miRNA-21 analysis, which shows a wide linear relationship and a low detection limit of 5.5 × 10−15 mol L−1. This study features the DNA intercalation-enabled organic electronics with superior gain and is envisaged to attract more attention to explore DNA adducts for innovative bioelectronics and biosensing, given the diverse DNA binders with multiple functions.
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Herein we report a high-gain signal-on poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) organic electrochemical transistor (OECT) biosensing using an accumulation-mode PEDOT:PSS ...OECT modulated by a light-fueled MXene/MOFs/NiO Schottky heterojunction. In such a system, the MXene/MOFs/NiO Schottky heterojunction exhibited superior gating effect, as it not only enabled the fast-directional charge transfer but also guaranteed the maximal accessibility of the electrolyte to topped 2D MXene with large surface area. In linkage with a bi-enzyme cascade system, the quinone derivatives produced by the cascade reaction of alkaline phosphatase (ALP) and tyrosinase (TYR) could serve as effective electron acceptors for the representative Ti
3
C
2
/PCN-224/NiO heterojunction, underpinning an innovative method for sensitive detection of ALP activity with a low detection limit of 0.001 U L
−1
. Remarkably, the as-developed system demonstrated a remarkable current gain as high as near 10
4
, which to our knowledge is the highest one among existing OECT biosensory devices. This work represents a generic protocol to develop the novel signal-on PEDOT:PSS OECT platform towards biochemical detection and beyond.
Within the context of residual cardiovascular risk in post-statin era, emerging evidence from epidemiologic and human genetic studies have demonstrated that triglyceride (TG)-rich lipoproteins and ...their remnants are causally related to cardiovascular risk. While, carriers of loss-of-function mutations of ApoC3 have low TG levels and are protected from cardiovascular disease (CVD). Of translational significance, siRNAs/antisense oligonucleotide (ASO) targeting ApoC3 is beneficial for patients with atherosclerotic CVD. Therefore, animal models of atherosclerosis with both hypercholesterolemia and hypertriglyceridemia are important for the discovery of novel therapeutic strategies targeting TG-lowering on top of traditional cholesterol-lowering. In this study, we constructed a novel mouse model of familial combined hyperlipidemia through inserting a human ApoC3 transgene (hApoC3-Tg) into C57BL/6 J mice and injecting a gain-of-function variant of adeno-associated virus-proprotein convertase subtilisin/kexin type 9 (AAV-PCSK9)-D377Y concurrently with high cholesterol diet (HCD) feeding for 16 weeks. In the last 10 weeks, hApoC3-Tg mice were orally treated with a combination of atorvastatin (10 mg·kg
·d
) and fenofibrate (100 mg·kg
·d
). HCD-treated hApoC3-Tg mice demonstrated elevated levels of serum TG, total cholesterol (TC) and low density lipoprotein-cholesterol (LDL-C). Oral administration of atorvastatin and fenofibrate significantly decreased the plaque sizes of en face aorta, aortic sinus and innominate artery accompanied by improved lipid profile and distribution. In summary, this novel mouse model is of considerable clinical relevance for evaluation of anti-atherosclerotic drugs by targeting both hypercholesterolemia and hypertriglyceridemia.
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