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In this study, a neoteric self-enhanced nanocomposite boron carbon nitride nanosheets (BCN NSs)-Ru obtained by chemical crosslinking between boron carbon nitride nanosheets (BCN NSs) and tris (4,4'-dicarboxylicacid-2,2'-bipyridyl) ruthenium(II) dichloride (Ru(dcbpy)

Herein, a multifunctional pentagon DNA nanostructure (MPDN) was assembled by the hybridization of a circular DNA scaffold containing five different fragments with five diverse DNA oligonucleotides for simultaneous sensitive detection and accurate colocalization imaging of dual-miRNAs in cancer cells. Exactly, the MPDN could specifically and efficiently internalize into folate (FA) receptor-overexpressed cells via specific binding of FA and the FA receptor to distinguish cancer cells from normal cells and transform trace amounts of targets miRNA-21 and miRNA-155 into substantial FAM and Cy5-labeled DNA polymers as the signal probe to generate two remarkable fluorescence emissions, realizing simultaneously sensitive detection of dual-miRNAs. Impressively, compared with traditional small fragment DNA probes with high fluidity, the DNA copolymers with extremely low diffusivity kept it in the originally generated position to achieve the colocalization imaging of dual-miRNAs more accurately for revealing the spatial expression information of dual-miRNAs in tissues and cells. This strategy provided programmable tool to simultaneously detect and accurately colocate dual-miRNAs for understanding normal physiology and the tumor mechanism.

Herein, a two-dimensional (2D) DNA structure with multiple ATP aptamers was elegantly designed to establish an electrochemical biosensor for rapid and sensitive detection of ATP based on ATP-induced structure switching. Concretely, the prepared 2D DNA structure containing numerous ATP aptamers as ATP-specific toehold switches could not only immobilize a large number of methylene blue (MB) for generating a remarkable electrochemical signal, but also greatly increase the local concentration of ATP aptamers to obviously enhance the capture efficiency of ATP. Once the target ATP interacted with the toehold switches, the 2D DNA structure could be sharply collapsed to trigger the burst release of MB from the electrode surface, ultimately resulting in a significantly decreased electrochemical signal for ultrasensitive detection of target ATP over a short period of time. Impressively, by dexterously adjusting the length of the ATP-specific toehold switches to 15-base, optimization of the binding affinity between ATP and the toehold switches was achieved for cutting down the detection time to 30 min and achieving a low detection limit of 0.3 pM, which addressed the shortcoming of time-consuming and poor sensitivity in the previous sensors with a small quantity of ATP aptamers and deficient binding affinity to ATP. Consequently, this strategy opened a promising avenue for ultrasensitive and rapid detection of various biomolecules in biomedical application and disease diagnosis.

In this work, a self-supplied electron photoelectrochemical (PEC) biosensor for sensitive determination of Pb

Herein, an innovative fluorescent sensor was courageously empoldered for precise and ultrasensitive detection and imaging of target miRNA-21 through the agency of a dextrous target-motivated polymerization/nicking DNA nanomachineries based on a hyperbranched rolling circle amplification (HB-RCA)-assisted multiposition strand displacement reaction (SDR) signal amplification approach. Impressively, the ingenious technique not only realized target recycling via polymerization/nicking DNA nanomachineries but also involved HB-RCA amplification induced by the released transformation target as the repeated signal amplification. Most importantly, HB-RCA was firstly exploited to remarkably increase the local concentration and collision efficiency of the templates and primers, which could simultaneously generate multiple repeated DNA sequences as initiators to supply substantial banding positions for SDR, removing the massive fluorescence-resonance-energy-transfer (FRET) DNA duplexes from the repeated DNA sequences to remarkably avert the self-quenching of the fluorescence signal due to self-aggregation caused by the winding of the HB-RCA products, thereby leading to a conspicuously improved signal amplification multiplier. As proof of concept, an ingenious technique effectively and accurately distinguished target miRNA-21 even with a tiny change in cells compared to the conventional fluorescence in situ hybridization (FISH) approach. Moreover, the proposed fluorescent method apparently discriminated drug-manipulative miRNA expression level abnormities. Therefore, the proposed cascade nucleic acid amplification strategy could provide an epigamic avenue for ultrasensitive imaging of diverse biomarkers, which help researchers to better study the tumor mechanism, thereby unambiguously increasing cancer cure rates and reducing the risk of recurrence.

Herein, a versatile ECL biosensor was fabricated for ultrasensitive detection of microRNA-21 (miRNA-21) from cancer cells based on a novel H2O2-free electrochemiluminescence (ECL) system (luminol/dissolved oxygen/Fe@Fe2O3 nanowires). Compared with the previously reported coreaction accelerator that needed a negative potential to produce reactive oxygen species (ROS), these newly discovered Fe@Fe2O3 nanowires could generate ROS in the detection solution immediately without the application of voltage, which narrowed down the detection potential range to avoid side reactions, favoring their practical application in biological systems. Especially, the Fe@Fe2O3 nanowires could produce H• for activating dissolved oxygen into ROS to improve the ECL intensity dramatically, which initiates a novel pathway to promote the generation of ROS for the ECL system. In addition, an original strand displacement amplification coupled with strand displacement reaction (SDA-SDR) was developed to improve the conversion efficiency of the target for sensitive detection of miRNA-21. By virtue of the SDR, a quadruple quenching effect was achieved through each output DNA strand of SDA; hence, the nucleic acid signal amplification efficiency was effectively enhanced. As expected, on account of the superb activation performance of Fe@Fe2O3 nanowires and the outstanding amplification efficiency of the SDR-SDA strategy, the fabricated ECL biosensor realized ultrasensitive detection of miRNA-21 with a detection limit down to 52.5 aM. The established ECL sensing platform ushered a new route for H2O2-free detection and a promising biomarker assay method for clinical diagnosis.

Herein, a photoelectrochemical (PEC) assay was designed for a highly sensitive DNA determination relying upon the SnO2/BiOBr p-n heterojunction as a photoactive material and SiO2 as a signal quencher. Compared with most traditional heterojunctions, the SnO2/BiOBr p-n heterostructure not only lessened the recombination of the photogenerated electron-hole pairs but also promoted the light-harvesting in the ultraviolet-visible (UV-vis) region, leading to further enhanced photoelectric conversion efficiency and photocurrent, which demonstrated 12.1-fold and 6.4-fold increments versus those of pure SnO2 and BiOBr, respectively. Additionally, the limited quantity of target DNA (a fragment of p53 gene) could be transformed into abundant output DNA-SiO2 by employing the Nt·BstNBI enzyme-assisted signal amplification procedure, leading to a highly improved detection sensitivity of the biosensor. Then, output DNA-SiO2 hybridized with the capture DNA anchored on the modified electrode surface, remarkably diminishing the PEC signal and thus achieving sensitive DNA determination. The elaborated PEC biosensor demonstrated outstanding performance within the linear range between 0.5 fM and 5 nM and a low limit of detection down to 0.18 fM, paving a new way for fabricating heterojunction with exceptional photoactive performance and demonstrating the enormous potential for detecting multitudinous biomarkers in bioanalysis and clinical therapy.

Herein, with skillfully engaging stable T-Hg2+-T bonding, a "Crab Claw"-like DNA nanomachine with concise and highly efficient assembly and enhanced recognition/conversion efficiency was engineered as a super signal amplifier, which was united with Pd@Cu@Pt multimetallic mesoporous nanomaterials (Pd@Cu@Pt MMNs) for ultrasensitive electrochemical assay of mercury ions (Hg2+). Specifically, the formed "Crab Claw"-like DNA nanomachine could simultaneously trigger four same cascade DNAzyme cleavage reactions with the help of Mg2+ DNAzyme for markedly converting target Hg2+ to enormous DNA segments labeled with ferrocene (Fc), improving the detection sensitivity. Subsequently, the prepared Pd@Cu@Pt MMNs could not only show commendable electrochemical catalysis to Fc but also act as an excellent immobilization matrix for capturing and accumulating abundant Fc around them to further strengthen the electrochemical signal. As a result, the well-designed electrochemical sensor could achieve a low limit of detection of 3.58 fM in the range from 10 fM to 100 nM for Hg2+detection. This strategy offers a simple and rapid avenue to detect heavy metal ions and shows promising application potential for environmental pollutant monitoring.

Ochratoxin A (OTA) with high toxicity represents a serious threat to the agriculture and food chain, consequently to human health. Herein, a simple electrochemiluminescence (ECL) biosensor was constructed for ultrasensitive detection of OTA based on mercaptopropionic acid templated Au nanoclusters (Au NCs) as intensive signal probe and a non-enzymatic 2D DNA walking machine as the effective amplification strategy. Specifically, the target related bipedal DNA walker efficiently moved along 2D DNA tracks through toehold-mediated DNA strand displacement, which triggered abundant signal probes for combining to the DNA tracks. Moreover, the Au NCs could exhibit strong ECL emission due to fast electron transfer from massive Au-S electronic pathways under the electrochemical excitation. Thus, the biosensor possessed significant ECL response for achieving ultrasensitive detection toward OTA with low detection limit of 3.19 fg/mL. Impressively, the sensing platform was also applied to detect OTA from edible oils, exhibiting great application potential in food analysis.

Herein, a supersensitive biosensor was constructed by using graphitic carbon nitride with a carbon vacancy (V

Aggregation-induced electrochemiluminescence (AIECL) has attracted extensive interest due to the significant increase in ECL response by restricting free intramolecular rotation and torsion, but traditional AIECL emitters suffer from limited ECL efficiency, high cost, and complex synthetic steps, dramatically limiting their applications. Herein, novel Al(III)-Cbatpy metal-organic gels (Al(III)-Cbatpy-MOGs) with nanofiber morphology and ultrarapid coordination of Al

Herein, a long period liner DNA tandem (Lr-DNT) was intelligently designed as DNA track for quadruped DNA walker (q-walker) to run in an orderly and efficient manner, which could be applied to construct an electrochemical biosensor for rapid and ultrasensitive detection of microRNA-21 (miRNA-21). Impressively, benefiting from the orderliness and equidistance of Lr-DNT, the q-walker could be endowed with a high controllability, directionality as well as a quite short reaction time down to 20 min compared with those of traditional DNA walkers walked on the stochastic tracks. Once the target miRNA-21 interacted with the locked q-walker, the q-walker could be activated to expeditiously cleave Lr-DNT for releasing amounts of signal probes ferrocene (Fc) with the assistance of the Nt.BbvCI enzyme. This way, the developed q-walker could not only readily overcome the problem of low reaction efficiency but also address the drawback of time consumption in a previous strategy. As a proof of concept, the prepared biosensor could accomplish sensitive detection of target miRNA-21 with a detection limit down to 31 aM. As a result, this tactic gave impetus to design high-performance sensing platform with ultimate application in clinical sample analysis and nucleic acid based cancer diagnostics.

Herein, an ultrasensitive and versatile electrochemical biosensor was developed through the target-controlled capture and release of signal probe-loaded DNA nanotube for the ultrasensitive detection of two different types of cancer-related biomarkers, microRNA-21 (miRNA-21) and glutathione (GSH). In this system, target 1 (miRNA-21) first triggered duplex-specific nuclease (DSN)-assisted recycle amplification to generate numerous disulfide-linked DNA strands (DL), which could effectively capture DNA nanotube to immobilize methylene blue (MB) to produce remarkable electrochemical signals and achieve the ultrasensitive detection of miRNA-21 with a detection limit down to 32.6 aM. Furthermore, in the presence of target 2 (GSH), the electrochemical signal was significantly reduced by a thiol-disulfide bond exchange reaction on DL to release MB-immobilized DNA nanotubes away from the sensing interface, which enabled the sensitive analysis of GSH with a detection limit of 0.379 nM. Impressively, this strategy could achieve ultrasensitive detection of different types of biomarkers to prominently lessen false-positive responses from the current sensing methods toward a single biomarker or the same type of biomarker and remarkably heighten the accuracy and precision of early cancer diagnosis. Meanwhile, the proposed electrochemical biosensor made it possible to realize the regenerative analysis of targets over four times without extra fuel, which could conspicuously improve the analytical efficiency compared with that of traditional biosensing assays. As a result, this study might open up novel insights to design a versatile and multifunctional sensing platform and encourage deeper exploration for detecting different types of biomarkers in the fields of early disease diagnosis and biochemical research.

Au nanoparticles (Au NPs) can be self-assembled in a bottom-up orderly manner at the oil-water interface, which is widely used as SERS platforms, but the stability of the Au NP interface needs to be improved due to shaking or shifting and the Brownian motion. The DNA structure with unique sequence specificity, excellent programmability, and flexible end-group modification capability owns good potential to precisely control the plasmonic structure's distance. In this study, a large area of the SERS substrate is obtained from the DNA structure-stabilized self-assembled ordered Au NPs on the cyclohexane-water interface. Combining with the exonuclease III (exo III)-assisted DNA recycling amplification strategy, we construct a liquid-phase SERS biosensor for efficient detection of microRNA 155 (miRNA 155). Compared with the traditional randomly assembled Au NPs on the two-phase interface, the SERS signal is significantly enhanced and more stable. The detection limit of the SERS biosensor for miRNA 155 reached 1.45 fmol/L, which has a very wide linear range (100 fmol/L-5 nmol/L). This work gives an efficient approach to stabilize the self-assembly Au NPs on the liquid-liquid interface, which can broaden the application of SERS analysis.

Herein, a novel Au nanoclusters/Cu2O (Au NCs/Cu2O) heterostructure exhibited exceptionally strong electrochemiluminescence (ECL) emission, in which the p-type semiconductor Cu2O was defined as the electrosensitizer to provide the electrogenerated holes for rapidly transferring the electrogenerated hot electrons of Au NCs. Thus, the fast charge transfer of Au NCs/Cu2O was achieved by the electrosensitizer compared to the sluggish one via intramolecular covalent bond charge transfer of traditional Au NCs, resulting in a greatly higher ECL efficiency (63.8%) than that of pure Au NCs (2.7%) versus the standard [Ru(bpy)3]2+. It solved one main challenge of electrochemiluminophore-based metal NCs: high efficiency with energic charge-transport kinetics. As a proof of concept, Au NCs/Cu2O was successfully employed in an ultrasensitive ECL biosensing platform for determining the biological antioxidant glutathione with a limit of detection (LOD) as low as 6.3 pM. The heterostructure as an ECL emitter is a very promising start for guiding the rational design of efficient electrochemiluminophores in intense light-emitting devices and high-definition ECL imaging.

Herein, a novel DNA cascade amplification, including double hairpin DNAs recognition-triggered single-target recycling (D-STR) and concatenated DNA structure-controlled rolling circle amplification (C-RCA), was developed as a signal amplifier to construct a highly specific and ultrasensitive electrochemiluminescence (ECL) biosensor for human immunodeficiency virus (HIV) DNA fragments detection, which not only revealed tremendous potential in avoiding false positive signals but also obviously promoted the amplification efficiency simultaneously compared to conventional single recognition of the target. Once the target DNA triggered the rolling circle amplification (RCA), the obtained RCA products could be anchored on the Pt-modified glassy carbon electrode (GCE) via the Pt-N bond, capturing massive ruthenium (Ru)-labeled ssDNA as the ECL signal tag to generate remarkable ECL emission. As a result, the proposed biosensor showed highly specific and ultrasensitive detection of the target with the detection limit down to 27.0 aM, which gives great impetus to the development of a novel specific biosensor for practical bioanalysis and diagnostic technologies.

Herein, a novel region recognition of precursor microRNA (Pre-miRNA) based on hyperbranched hybrid chain reaction (HB-HCR) amplification was constructed to effectively eliminate the interference of Pre-miRNA to the mature microRNA (miRNA) by establishing the linear mapping relation between the two fluorescence signals produced by the miRNA sequence in the Pre-miRNA and Pre-miRNA residues to first realize simultaneous sensitive detection of Pre-miRNA and miRNA as well as highly sensitive imaging of intracellular Pre-miRNA and miRNA, which solves one main challenge of

A highly loaded and integrated core–brush three-dimensional (3D) DNA nanostructure is constructed by programmatically assembling a locked DNA walking arm (DA) and hairpin substrate (HS) into a repetitive array along a well-designed DNA track generated by rolling circle amplification (RCA) and is applied as a 3D DNA nanomachine for rapid and sensitive intracellular microRNA (miRNA) imaging and sensing. Impressively, the homogeneous distribution of the DA and HS at a ratio of 1 : 3 on the DNA track provides a specific walking range for the DA to avoid invalid and random self-walking and notably improve the executive ability of the core–brush 3D DNA nanomachine, which easily solves the major technical challenges of traditional Au-based 3D DNA nanomachines: low loading capacity and low executive efficiency. As a proof of concept, the interaction of miRNA with the 3D DNA nanomachine could initiate the autonomous and progressive operation of the DA to cleave the HS for ultrasensitive ECL detection of target miRNA-21 with a detection limit as low as 3.57 aM and rapid imaging in living cells within 15 min. Therefore, the proposed core–brush 3D DNA nanomachine could not only provide convincing evidence for sensitive detection and rapid visual imaging of biomarkers with tiny change, but also assist researchers in investigating the formation mechanism of tumors, improving their recovery rates and reducing correlative complications. This strategy might enrich the method to design a new generation of 3D DNA nanomachine and promote the development of clinical diagnosis, targeted therapy and prognosis monitoring., This study designed a highly loaded and integrated core–brush 3D DNA nanomachine for miRNA imaging and sensing, which easily solves the major technical challenges of traditional Au-based 3D nanomachines: low loading capacity and low executive efficiency.

Herein, a novel co-catalytic ferrocene/hemin/G-quadruplexes/Fe3O4 nanoparticles (Fc/HGQs/Fe3O4) nanocomposite was synthesized to significantly magnify the electrochemical signal of ferrocene (Fc) using the synergistic catalysis of hemin/G-quadruplexes (HGQs) and Fe3O4 nanoparticles as hydrogen peroxide enzyme mimics for the construction of ultrasensitive electrochemical biosensors. The fabricated electrochemical biosensor can achieve ultrasensitive detection of miRNA-155 ranging from 0.1 fM to 1 nM, as well as a limit of detection of 74.8 aM. This strategy provides a new route to exploring efficient signal labels for signal amplification and provides an impetus to find novel methods for the construction of biosensors for biological detection and the early clinic diagnosis of diseases.

Molybdenum dioxide (MoO2) suffers from large volume expansion and poor conductivity as anode material for lithium ion battery (LIB). Herein, the three-dimensional (3D) MoO2/N-doped carbon composites constructed by amorphous nanowires and crystalline nanoparticles (marked as 3D MoO2/NC composites) are prepared. It is worth mentioning that the conductivity could be largely improved as well as the volume expansion could be effectively relieved since the structure design including amorphous, carbon-composited and pony-size are taken, resulting in high Li storage capacity of MoO2. Benefiting from the especial structural feature, the 3D MoO2/NC composites exhibit an excellent electrochemical performance compared to the pristine crystalline MoO2 and display a higher capacity of 912 mAh g−1 after 250 cycles at 0.1 A g−1. The proposed structure design can be reference to prepare other electrode materials for boosting the Li storage properties.

The design of photoactive materials is critical for enhancing the performance of photoelectrochemical (PEC) sensing platforms. In this work, a novel tungsten-doped In2S3 (In2S3:W) nanostructure with excellent PEC performance (six-fold enhancement compared to the pristine In2S3:W) was prepared by a dissolution–regrowth process for ultrasensitive biosensing. We show that the high-valence dopant W4+ in the In2S3 material introduced impurity energy levels and defects that can improve the separation of photo-carriers and therefore enhanced the PEC performance. This mechanism was also confirmed by density functional theory calculations. The designed defective In2S3:W material offers a highly active and stable platform for PEC applications. By using the In2S3:W material as a signal indicator, a PEC sensing platform for cancer biomarkers, vascular endothelial growth factor (VEGF165), was established with the assistance of the target-induced exponential amplification reaction and enzymatic biocatalytic precipitation reaction. The results demonstrated that the PEC sensor exhibited excellent performance with a sensitivity of 0.3 fM due to the high initial PEC signal and photo-carrier separation efficiency of In2S3:W. This work gives an in-depth understanding of the enhancement of PEC performance by defect engineering and provides a new PEC sensing platform for bioanalysis and diagnosis.

In this work, a tetrahedral DNA nanostructure (TDN) designed with multiple biomolecular recognition domains (m-TDN) was assembled to construct an ultrasensitive electrochemical biosensor for the quantitative detection of tumor-associated mucin 1 (MUC-1) protein. This new nanostructure not only effectively increased the capture efficiency of target proteins compared to the traditional TDN with a single recognition domain but also enhanced the sensitivity of the constructed electrochemical biosensors. Once the target MUC-1 was captured by the protein aptamers, the ferrocene-marked DNA strands as electrochemical signal probes at the vertices of m-TDN would be released away from the electrode surface, causing significant reduction of the electrochemical signal, thereby enhancing significantly the detection sensitivity. As a result, this well-designed biosensor achieved ultrasensitive detection of the biomolecule at a linear range from 1 fg mL

Herein, the boron radical active sites of boron carbon oxynitride quantum dots (BCNO QDs) are electrically excited to produce boron radicals (B•) for catalyzing peroxydisulfate (S2O82-) as a coreactant to accelerate the generation of abundant sulfate radicals (SO4•-) for significant enhancement in the electrochemiluminescence (ECL) efficiency of BCNO QDs, which overcome the defect of traditional carbon-based QDs with low ECL efficiency. Impressively, under extremely low concentration of S2O82- solution, the BCNO QDs/S2O82- system could exhibit high ECL emission, realizing environmental friendliness and excellent biocompatibility for sensitive bioanalysis. As a proof-of-concept, BCNO QDs, a new generation of ECL emitters with high ECL efficiency, were successfully used in the ultrasensitive determination of microRNA-21, which pushes the exploration of new ECL emitters and broadens the application in the field of clinical diagnosis, ECL imaging, and molecular devices.

Herein, a novel single-enzyme-assisted dual recycle amplification strategy based on T7 exonuclease (T7 Exo) and a strand-displacement reaction (SDR) was designed to fabricate a photoelectrochemical (PEC) biosensor for sensitive microRNA-141 (miRNA-141) detection with the use of laminar bismuth tungstate (Bi2WO6) as photoactive material. Compared with a traditional enzyme-assisted dual recycle amplification strategy, the presented method could effectively refrain the enzyme interference reaction, reduce environmental sensitivity, and save cost. Here, hairpin DNA1 (H1) decorated on magnetic beads (MB) hybridized with target miRNA-141 to form an H1/miRNA-141 heteroduplex. With the introduction of hairpin DNA2 (H2)-labeled SiO2 (H2-SiO2), SDR was triggered between H2-SiO2 and H1, thus miRNA-141 was displaced from the H1/miRNA-141 heteroduplex and an H1/H2-SiO2 duplex was formed, realizing the reuse of the target. In the presence of T7 Exo, the H1/H2-SiO2 duplex was digested with the release of output DNA-SiO2. To enhance the target conversion rate, H1-MB was intactly released and cycled, which could initiate more T7 Exo digestion and free abundant output DNA-SiO2. Through such a process, a tiny miRNA-141 could induce substantial output DNA-SiO2, effectively improving the target amplification efficiency and detection sensitivity of a PEC biosensor. Furthermore, Bi2WO6 was modified on an electrode to provide a superior initial PEC signal due to its excellent electronic transformation capacity. With the introduction of output DNA-SiO2, the hairpin structure of H3 on the electrode was opened, making SiO2 close to the electrode surface, which significantly decreases the PEC signal. This work first established the PEC biosensor featuring a single-enzyme-assisted dual recycle amplification process for sensitive detection of biomarkers.

Copper nanoclusters (Cu NCs) as emerging luminescent metal NCs are gaining increasing attention owing to the comparatively low cost and high abundance of the Cu element in nature. However, it remains challenging to manipulate the optical properties of Cu NCs. Unlike most dispersed Cu NCs, whose luminescence efficiency was restricted by nonexcited relaxation, the Cu NCs confined in a porous poly-l-cysteine (poly-l-Cys) film were generated controllably with enhanced electrochemiluminescence (ECL) by in situ electrochemical reduction. Specifically, poly-l-Cys provided a porous structure to regulate the generation of Cu NCs within its holes, which not only increased the restriction on the intramolecular vibration and rotation of the ligands but also expedited the electron transfer near the electrode surface, reflecting in an enhancement of the ECL signal and efficiency. As an application of the confined Cu NCs, an ECL biosensor with high performance was constructed skillfully for highly sensitive detection of alkaline phosphatase (ALP), which adopted Cu NCs as the ECL luminophore and poly-l-Cys as a coreaction accelerator in a novel ECL ternary system (Cu NCs/S2O82-/poly-l-Cys). Furthermore, an ingenious target amplification based on the combination of a DNA walker and click chemistry was developed to convert ALP to DNA strands efficiently, achieving great improvement in the recognition efficiency. As a result, the biosensor had a low detection limit (9.5 × 10-7 U·L-1) and a wide linear range (10-8-10-2 U·L-1) for ALP detection, which showed great promise for the detection of non-nucleic acid targets and the diagnosis of diseases.

Herein, an orbitron-like three-dimensional (3D) DNA clip-based nanomachine was proposed for ultrasensitive fluorescent bioassay of microRNA, which was constructed by mechanically interlocking double-DNA-ring with two single-stranded DNAs, performing an orbitron-like 3D structure with double freely rotated DNA rings as the open state. In the presence of target microRNA, the proposed orbitron-like 3D DNA clip can alter its structure from open to closed state in identification of the target microRNA, generating the closure between the previously modified fluorescent dyes and the quenchers to perform a "signal off" fluorescent signal correlated with the concentration of target microRNA. Compared with the normal DNA nanomachines, such as DNA tweezers constructed by self-assembly of three single-stranded DNAs which regulated the open and closed states on the basis of linear conformational changes, the proposed 3D DNA clip-based nanomachine with high mechanical rigidity realized the conformational changes in 3D space with the assistance of target microRNA, which could effectively increase the adjustable distance range and reduce the background signal. Furthermore, the 3D DNA clip-based nanomachine was applied in the fluorescent detection of microRNA-21 with favorable performances for the sensitive detection of microRNA in cells, providing a new avenue for early clinical diagnoses of disease.

Herein, an amphiphilic perylene derivative (denoted as PTC-DEDA) was explored as DNA intercalators endowed with an enhanced affinity and intense electrochemiluminescence (ECL) to construct a target-induced DNA hydrogel biosensing platform for the sensitive detection of microRNA let-7a (miRNA let-7a). Specifically, the DNA hydrogel with numerous dendritic DNA structures was in situ generated

The evident contradiction between high local-concentration-based substrate reactivity and free-diffusion-based high reaction efficiency remains one of the important challenges in chemistry. Herein, we propose an efficient aggregation-induced synergism through the hydrophobic-driven self-assembly of amphiphilic oligonucleotides to generate high local concentration whereas retaining high reaction efficiency through hydrophobic-based aggregation, which is important for constructing efficient DNA nanomachines for ultrasensitive applications. MicroRNA-155, used as a model, triggered strand displacement amplification of the DNA monomers on the periphery of the 3D DNA nanomachine and generated an amplified fluorescent response for its sensitive assay. The local concentration of substrates was increased by a factor of at least 9.0×105 through hydrophobic-interaction-based self-assembly in comparison with the traditional homogeneous reaction system, achieving high local-concentration-based reactivity and free-diffusion-based enhanced reaction efficiency. As expected, the aggregation-induced synergism by hydrophobic-driven self-assembly of amphiphilic oligonucleotides created excellent properties to generate a 3D DNA nanomachine with potential as an assay for microRNA-155 in cells. Most importantly, this approach can be easily expanded for the bioassay of various biomarkers, such as nucleotides, proteins, and cells, offering a new avenue for simple and efficient applications in bioanalysis and clinical diagnosis.

Synthesis of a highly efficient electrochemiluminescence (ECL) luminescent material is one of the effective means to improve the sensitivity of the sensor. In this study, an efficient ECL luminescent nanomaterial, carbon nitride nanosheet (CNNS) decorated amino-functional metal-organic frameworks (CNNS@NH2-MIL(Fe)) were synthesized for sensitive ECL detection of cardiac troponin I (cTn-I). The synthesized CNNS@NH2-MIL(Fe) realized the effective mass loading of CNNS, and more importantly, the NH2-MIL(Fe) could expedite the reduction of coreactant S2O82- to produce abundant ECL reaction intermediate SO4•- near CNNS, thus, shortening the distance between SO4•- and the excited state of CNNS with less energy loss to extremely enhance the ECL signal of CNNS. Furthermore, the ECL signal of the immunosensor could be further enhanced when the Ti3C2 nanosheet was used as the matrix to capture primary anti-cTn-I due to the reason that Ti3C2 not only exhibited a large surface area and excellent metallic conductivity, but also could act as a coreaction accelerator to speed up the reduction of S2O82- with plenty of SO4•- generated. Therefore, this proposed ECL immunosensor using CNNS@NH2-MIL(Fe) as a signal probe and Ti3C2 as a sensing matrix exhibited a significantly enhanced ECL signal and had a high sensitivity and excellent selectivity for cTn-I. Consequently, this multiple signal amplification strategy provided an effective method for trace protein ultrasensitive detection in ECL bioanalysis.

In this work, Bi2Te3 nanosheets treated with N-vinyl-pyrrolidinone showed highly sufficient and stable photocurrent for being used as a novel photoactive material. Accordingly, with CdTe quantum dots (QDs) sensitizing Bi2Te3 nanosheets, photoelectrochemical (PEC) biosensor coupling of DNA-amplifying strategies was constructed for sensitive miRNA-21 detection. Initially, the Bi2Te3 nanosheets on the electrode have conductive surface states with dissipationless electronic property, thus providing a highly stable photocurrent and a large surface-to-volume ratio. Then, with the participation of target miRNA-21 and auxiliary DNA, strand displacement amplification took place, thereby opening substantial DNA hairpins for triggering the next hybridization chain reaction (HCR). Through the HCR, long DNA tails decorated with CdTe QDs could thus be assembled on the electrode for enhancing the photocurrent of Bi2Te3 nanosheets. As a result, the proposed PEC biosensor showed a wide detection range from 10 fM to 100 pM with a detection limit of 3.3 fM, displaying a promising avenue to construct simple, ultrasensitive, and stable analytical techniques and tremendous potential in bioanalysis and early clinical diagnosis.

Here we described an effective recognition strategy using the target-triggered DNA structure transition as an affinity switch for nucleic acid detection based on the strong electrochemiluminescence (ECL) platform of 9,10-diphenylanthracene (DPA) doped perylene (Pe) microcrystals (DPA@Pe MCs). Specifically, the target-triggered rolling-circle amplification (RCA) could generate a long, single-stranded DNA with repeated G-quadruplex units, which would hinder the access of quenching probes due to the steric hindrance effects offered by the DNA structure transition. Using this effective recognition strategy, an ECL biosensor with ultrasensitive and accurate characteristics was proposed to detect microRNA-21, which showed an excellent linear response from 10 aM to 1 pM with the detection limit down to 4.14 aM. The DNA structure transition-induced affinity switch strategy offered a potential applications in clinical diagnosis analysis.

Herein, a Janus three-dimensional (3D) DNA nanomachine was constructed for the simultaneous and sensitive fluorescence detection and imaging of dual microRNAs (miRNAs) in cancer cells, which could effectively eliminate signal interference in a homogeneous nanoparticle-based 3D DNA nanostructure caused by the proximity of the two different signal probes to achieve accurate co-location in the same position of living cancer cells. In this system, the Janus nanoparticles were synthesized as the carrier for immobilizing two different oligonucleotides on two different functionalized hemispheres of the nanoparticles to form a Janus 3D DNA nanostructure, which could convert trace amounts of miRNA-21 and miRNA-155 targets into massive FAM and Cy5-labeled duplexes to induce two remarkable fluorescence emissions by the catalytic hairpin assembly (CHA) and 3D DNA walker cascade nucleic acid amplification strategy, realizing sensitive detection and imaging of miRNA targets in cancer cells. Impressively, in comparison with current miRNA imaging methods based on nanoparticle assemblies, the proposed strategy could efficiently eliminate “false positive” results obtained in single type miRNA detection and distinctly increase the immobilization concentration of two different signal probes using Janus nanoparticles as the carrier to further enhance fluorescence intensity, resulting in accurate co-location in the same position of living cells. Meanwhile, the proposed fluorescence imaging technology makes it possible to visualize low concentrations of miRNAs with tiny change associated with some cancers, which could significantly improve the accuracy and precision compared to those of the conventional fluorescence in situ hybridization (FISH) approach. Therefore, it could serve as persuasive evidence for supplying accurate information to better understand biological processes and investigate mechanisms of various biomolecules and subcellular organelles, resulting in the further validation of their function in tumor proliferation and differentiation. This strategy provided an innovative approach to design new generations of nanomachines with ultimate applications in bioanalysis and clinical diagnoses., A Janus three-dimensional DNA nanomachine was constructed for the simultaneous and sensitive fluorescent detection and imaging of dual microRNAs in the cancer cells.

Electrochemiluminescence (ECL) micro-reactors with enhanced intensity and extreme stability were first established by the assembly of tris(2,2′-bipyridyl) ruthenium(ii) (Ru(bpy)32+) onto covalent organic frameworks (COFs), in which a type of imine-linked COF (denoted as COF-LZU1) was employed as a model for ECL micro-reactors. Compared with the dominant ECL system of Ru(bpy)32+/tri-n-propylamine (TPrA) (TPrA as a co-reactant), the intensity of the COF-LZU1 micro-reactor-based electrode was significantly increased nearly 5-fold under the same experimental conditions, which is unprecedented in other Ru(bpy)32+-based ECL systems. This enhancement can be attributed to the large surface area, delimited space, and stable and hydrophobic porous structure of COF-LZU1, which not only enabled a huge amount of Ru(bpy)32+ to be loaded in/on COF-LZU1, but also enriched a large amount of TPrA from the aqueous solution into its inner hydrophobic cavity due to the lipophilicity of TPrA. More importantly, with its hydrophobic porous nanochannels, COF-LZU1 could act as micro-reactors to provide a delimited reaction micro-environment for the electrochemical oxidation of TPrA and the survival of TPrA˙, achieving significant confinement-enhanced ECL. To prove this principle, these Ru@COF-LZU1 micro-reactors were developed to prepare an ECL aptasensor for aflatoxin M1 (AFM1) detection with a wide detection range and a low detection limit. Overall, this work is the first report in which ECL micro-reactors are constructed with COFs to enhance the intensity and stability of the Ru(bpy)32+-based ECL system, and opens a new route to the design of other ECL micro-reactors for bioanalysis applications., The electrochemiluminescence (ECL) micro-reactors with enhanced intensity and extreme stability were firstly established, unravelling the mechanism of ECL micro-reactors using COF-LZU1 assembled Ru(bpy)32+ as a case study.

A kind of organic microcrystal, 9,10-diphenylanthracene microcrystals (DPA MCs), was developed as a novel electrochemiluminescence (ECL) coreactant accelerator to efficiently catalyze dissolved O2 for more reactive oxygen species (ROSs) generation, achieving intense ECL for a H2O2-free luminol system. Moreover, based on this ternary ECL system, a signal "off-on" ECL biosensor for microRNA-21 (miRNA-21) detection was constructed combining a sensitive target recycling amplification strategy and an enzyme-mediated recycling strand displacement reaction (RSDR).

We report the synthesis of phosphorus-doped ZnIn2S4 (ZnIn2S4-xPx) materials through a solid/gas-phase reaction. ZnIn2S4-xPx shows enhanced photoelectrochemical (PEC) performance due to the improved photo-carrier separation efficiency achieved by substituting some of the sulfur with phosphorus. A PEC biosensor was further developed based on ZnIn2S4-xPx, which exhibits excellent analytical performance for miRNA-155.

By using multivalent manganese oxides microflowers (MnOx MFs) as prominent a coreaction accelerator in luminol/dissolved oxygen system, and by combining these with DNA nanostructures for efficient immobilization of the electrochemiluminescence (ECL) quencher doxorubicin-ferrocenecarboxylic acid (Dox-FcCOOH), an ultrasensitive biosensing platform was constructed to conduct a microRNA assay in tumour cells.

In this work, a novel DNA nanostructure with a shorter assembly time and larger loading capacity was constructed using amphiphilic DNA-alkane group (Spacer C12)10 conjugates encapsulating plentiful fat-soluble fluorescent dyes into the hydrophobic core to form the DNA micelles, which could be rapidly self-disassembled via target induced hydrophilic-hydrophobic regulation to release fluorescent dyes from micelles to the organic phase, realizing the fast and sensitive detection of microRNA.

Herein, we report a three-dimensional (3D) DNA walking nanomachine innovatively constructed from a functionalized 3D DNA track, which runs in an orderly manner with favorable directionality to allow for programming certain pathways of information transduction for some target tasks. The nanomachine was constructed using a departure station of walker (UB + W) and a functionalized 3D track, which was made up of a rolling circle amplification (RCA)-generated backbone chain and numerous triangular rung units with stators (UA + S) assembled into a repeating array along the backbone. A specific domain (SD) was designed at the 5′-end of the backbone to capture the UB + W, and stators with specific RNA substrates were immobilized at the three UA corners for the DNA walker to travel on. Powered by 10–23 DNAzyme, the DNA walker started moving from the SD end to the other end of the track by the autonomous cleavage of RNA substrates. Significantly, the homogeneous distribution of stators in the longitudinal and horizontal extensions paved a specific path for each walker to move along the 3D track. This resulted in random and inactive self-avoiding walking; thus, the nanomachine exhibited good executive ability. These properties allowed the DNA walking nanomachine to program the certain pathways of information transduction for the stepwise and programmed execution of some target tasks, such as the synthesis of specific polyorganics and cargo delivery. We believe that such a 3D DNA walking nanomachine could enrich the concept in the field of dynamic DNA nanotechnology, and may improve the development of novel DNA nanomachines in cargo delivery and composite product synthesis., A three-dimensional DNA walking nanomachine innovatively constructed from a functionalized 3D DNA track which runs in an orderly manner with favorable directionality.

The sensitivity of cathodic photoelectrochemical (PEC) biosensor is mainly limited by the weak photocurrent response of p-type semiconductors due to the intrinsic weak hole conduction and severe charge recombination. Herein, we developed an antenna-like strategy that can amplify 10-fold of the cathodic photocurrent without using of p-type semiconductor. Specifically, poly (3,4-ethyl-enedioxythiophene) (PEDOT) was used as photocathode to improve the migration of photo-generated electrons (e