Study on the Electrochemiluminescence Emission Mechanism of HOF-14 and Its Multimode Sensing and Imaging Application.

A novel hydrogen-bonded organic framework (HOF-14) has attracted much attention due to its excellent biocompatibility and low toxicity, but its research in the electrochemiluminescence (ECL) field has not been reported. In this work, the annihilation-type and coreactant-type ECL emission mechanisms of HOF-14 were studied systematically for the first time. It was found that the ECL quantum efficiency of HOF-14/TEA coreactant system was the highest, which was 1.82 times that of Ru(bpy)32+/TEA. Further, the ECL emission intensity of HOF-14/TEA system could achieve colorimetric (CL) imaging of mobile phone. We also discovered that HOF-14 had superior photoelectrochemical (PEC) performance. Based on the above research results, a unique HOF-14-based multimode sensing and imaging platform was constructed. The antibiotic Enrofloxacin (ENR) was selected as the detection target, and the Cu-Zn bimetallic single-atom nanozyme (Cu-Zn/SAzyme) with excellent peroxidase (POD)-like activity was used to prepare quenching probes. When the target ENR was present, Cu-Zn/SAzyme quenching probes were introduced to the surface of HOF-14 by the dual-aptamer sandwich method. Cu-Zn/SAzyme could catalyze diaminobenzidine (DAB) to produce brown precipitations to quench the ECL, PEC, and CL signals of HOF-14, realizing multimode detection of ENR. This work not only discovered excellent ECL and PEC property of new HOF-14 material but also systematically studied the ECL emission mechanism of HOF-14, and proposed a novel multimode sensing and imaging platform, which greatly improved the detection accuracy of target and showed great contributions to the field of ECL analysis.

Zero-Background Dual-Mode Closed Bipolar Electrode Electrochemiluminescence Biosensor Based on ZnCoN-C Potential Regulation for Ultrasensitive Detection of Ochratoxin A.

In this work, the relationship between electrochemiluminescence (ECL) signal and driving voltage was first studied by self-made reduced and oxidized closed bipolar electrodes (CBPEs). It was found that when the driving voltage was large enough, the maximum ECL signals for the two kinds of CBPEs were the same but their required drive voltages were different. Zinc cobalt nitrogen doped carbon material (ZnCoN-C) had an outstanding electric double layer (EDL) property and conductivity. Therefore, it could significantly reduce the driving voltage of two kinds of CBPE systems, reaching the maximum ECL signal of Ru(bpy)32+. Interestingly, when the ZnCoN-C modified electrode reached the maximum ECL signal, the bare electrode signal was zero. As a proof-of-concept application, a zero-background dual-mode CBPE-ECL biosensor was constructed for the ultrasensitive detection of ochratoxin A (OTA) in beer. Considering that beer samples contained a large number of reducing substances, a reduced CBPE system was selected to build the biosensor. Furthermore, a convenient ECL imaging platform using a smartphone was built for the detection of OTA. This work used a unique EDL material ZnCoN-C to regulate the driving voltage of CBPE for the first time; thus, a novel zero-background ECL sensor was constructed. Further, this work provided a deeper understanding of the CBPE-ECL system and opened a new door for zero-background detection.

Spatial-Potential-Color-Resolved Bipolar Electrode Electrochemiluminescence Biosensor Using a CuMoOx Electrocatalyst for the Simultaneous Detection and Imaging of Tetracycline and Lincomycin.

A spatial-potential-color-resolved bipolar electrode electrochemiluminescence biosensor (BPE-ECL) using a CuMoOx electrocatalyst was constructed for the simultaneous detection and imaging of tetracycline (TET) and lincomycin (LIN). HOF-101 emitted peacock blue light under positive potential scanning, and CdSe quantum dots (QDs) emitted green light under negative potential scanning. CuMoOx could catalyze the electrochemical reduction of H2O2 to greatly increase the Faradic current of BPE and realize the ECL signal amplification. In channel 1, CuMoOx-Aptamer II (TET) probes were introduced into the BPE hole (left groove A) by the dual aptamer sandwich method of TET. During positive potential scanning, the polarity of BPE (left groove A) was negative, resulting in the electrochemical reduction of H2O2 catalyzed by CuMoOx, and the ECL signal of HOF-101 was enhanced for detecting TET. In channel 2, CuMoOx-Aptamer (LIN) probes were adsorbed on the MXene of the driving electrode (DVE) hole (left groove B) by hydrogen-bonding and metal-chelating interactions. LIN bound with its aptamers, causing CuMoOx to fall off. During negative potential scanning, the polarity of DVE (left groove B) was negative and the Faradic current decreased. The ECL signal of CdSe QDs was reduced for detecting LIN. Furthermore, a portable mobile phone imaging platform was built for the colorimetric (CL) detection of TET and LIN. Thus, the multiple mode-resolved detection of TET and LIN could be realized simultaneously with only one potential scan, which greatly improved detection accuracy and efficiency. This study opened a new technology of BPE-ECL sensor application and is expected to shine in microchips and point-of-care testing (POCT).

Potential-Resolved Ratio Electrochemiluminescence Biosensor Based on Perylene Diimide-MOF and DNA Nanoflowers-CdS Quantum Dots for Detection of Dual Targets.

BRCA1 gene and carcinoembryonic antigen (CEA) are important markers of breast cancer, so accurate detection of them is significant for early detection and diagnosis of breast cancer. In this study, a potential-resolved ratio electrochemiluminescence (ECL) biosensor using perylene diimide (PDI)-metal-organic framework and DNA nanoflowers (NFs)-CdS quantum dots (QDs) was constructed for detection of BRCA1 and CEA. Specifically, PDI-MOF and CdS QDs can generate potential-resolved intense ECL signals only using one coreactant, so the detection procedure can be effectively simplified. PDI-MOF was first attached to the electrode by graphene oxide, and the dopamine (DA) probe was linked to quench the ECL signal by DNA hybridization. In the presence of target BRCA1, it can form a bipedal DNA walker, so the quenching molecules (DA) were detached from the electrode via the walker amplification process aided by Mg2+, so that the PDI signal at -0.25 V was restored for the BRCA1 assay. Moreover, CdS QDs@DNA NFs as amplified signal probes were formed by self-assembly, and the target CEA-amplified product introduced the CdS QDs@DNA NFs to the electrode, so the QD ECL signal at -1.42 V was enhanced, while the ECL signal of PDI is unchanged; thus, CEA detection was achieved by the ratio value between them. Therefore, the detection accuracy is guaranteed by detection of two cancer markers and a ratio value. This biosensor has a great contribution to the development of new ECL materials and a novel ECL technique for fast and efficient multitarget assays, showing great significance for the early monitoring and diagnosis of breast cancer.

Multifunctional Photoelectrochemical Biosensor Based on ZnIn2S4/ZnS QDs@Au-Ag-Reversed Photocurrent of Cu-Metal-Organic Framework Coupled with CRISPR/Cas-12a-Shearing for Assay of Dual Targets.

False positives and negatives in bioanalytical assays remain a persistent problem. Herein, a multifunctional photoelectrochemical (PEC) biosensor based on ZnIn2S4 (ZIS)/ZnS quantum dots (QDs)@Au-Ag-reversed photocurrent of Cu-metal-organic framework (MOF) coupled with CRISPR/Cas-12a-shearing was innovatively developed for assay of dual targets. First, Cu-MOF as a good PEC material shows cathodic photocurrent. Then, numerous ZIS/ZnS QDs were assembled to the Au-Ag nanoparticles (NPs) to prepare a stable and highly amplified signal probe, which can just match the energy level of Cu-MOFs and realized the polarity-reversed photocurrent of Cu-MOF for the first time. As the empty-core nanostructure of Au-Ag NPs has a high specific surface area and low material density, the bimetallic nanocrystal can much increase the reaction rate and improve the redox efficiency. When target CEA-produced cDNA opened the hairpin DNA (HP1 DNA) on the electrode, the ZIS/ZnS QDs@Au-Ag signal probe was conjugated to the electrode via DNA hybridization, achieving a significantly reversed PEC current for CEA detection. Moreover, the specific binding of kanamycin/aptamer generated the acDNA (activator), which can activate the trans-cleavage activity of the CRISPR-CAS12a system on ssDNA, so the signal probe was sheared and caused the obvious decrease of PEC signal for kanamycin detection. The newly developed ZIS/ZnS QDs@Au-Ag NPs displayed excellent PEC properties and reversed photocurrent to MOF and were combined with the unique CRISPR-Cas12a system to achieve sensitive detection of dual targets, which can open a new polarity-reversed PEC sensing platform for rapid and accurate analysis of multiple targets and can effectively avoid false positives results in clinical testing.

A novel DNA-quantum dot nanostructure electrochemiluminescence aptamer sensor by chain reaction amplification for rapid detection of trace Cd2.

This work proposes a new enzyme-free electrochemiluminescence (ECL) sensing platform based on a novel DNA-quantum dot (QD) nanostructure and hybridization chain reaction (HCR) amplification for the trace detection of Cd2+. First, the Cd2+ aptamer triggers the HCR amplification circuit, so abundant biotin-labeled DNAs are introduced to the electrode, and then biotin as a linker specifically captures a large number of streptavidin (SA)-CdS QD complexes, showing very high ECL signals. After the present Cd2+ binds to its aptamer on the electrode, it causes the linear DNA structure loaded with a large number of QDs to break away from the electrode, resulting in a significantly decreased ECL response. This method combines the HCR-amplified DNA structure-QD signal with the specificity of the biotin-avidin reaction, enabling the rapid detection of Cd2+ in complex water. Therefore, this sensor provides a novel and competitive strategy for detecting heavy metal ions in actual samples, which extends its application to practical settings, such as environmental monitoring and biomedical diagnostics.

A multifunctional electrochemiluminescence and photoelectrochemical biosensor based on a quantum dot ion-exchange reaction for two-channel detection of thrombin.

Herein, a multifunctional electrochemiluminescence (ECL) and photoelectrochemical (PEC) biosensor based on exchange of Ag+ with CdTe QDs was developed for dual-mode detection of thrombin. First, CdTe QDs assembled on an electrode displayed superior ECL and PEC signals. At the same time, C-rich hairpin (HP) DNA linked to silicon spheres loaded a large amount of Ag+, and the specific binding of thrombin to an aptamer led to the release of DNA P; then, DNA P interacted with HP DNA to produce numerous Ag+ ions by an enzyme-digestion amplification reaction. Ag+ underwent ion exchange with CdTe QDs to generate AgTe/CdTe QDs, resulting in much reversed PEC and changed ECL signals for dual-mode detection of thrombin. This work takes advantage of outstanding multi-signals of QDs coupled with convenient ion exchange to achieve multi-mode detection of the target, avoiding false positive or false negative signals generated in the traditional detection process, and thus can be used for the rapid detection of various biomolecules in actual samples.

Versatile Photoelectrochemical Biosensing for Hg2+ and Aflatoxin B1 Based on Enhanced Photocurrent of AgInS2 Quantum Dot-DNA Nanowires Sensitizing NPC-ZnO Nanopolyhedra.

Eliminating false positives or negatives in analysis has been a challenge. Herein, a phenomenon of polarity-switching photocurrent of AgInS2 quantum dot (QD)-DNA nanowires reversing nitrogen-doped porous carbon-ZnO (NPC-ZnO) nanopolyhedra was found for the first time, and a versatile photoelectrochemical (PEC) biosensor with a reversed signal was innovatively proposed for dual-target detection. NPC-ZnO is a photoactive material with excellent PEC properties, while AgInS2 QDs as a photosensitive material match NPC-ZnO in the energy level, which not only promotes the transfer of photogenerated carriers but also switches the direction of PEC current. Furthermore, in order to prevent spontaneous agglomeration of AgInS2 (AIS) QDs and improve its utilization rate, a new multiple-branched DNA nanowire was specially designed to assemble AgInS2 QDs for constructing amplified signal probes, which not only greatly increased the load of AgInS2 QDs but also further enhanced the photoelectric signal. When the target Hg2+-induced cyclic amplification process generated abundant RDNA, the DNA nanowire signal probe with plenty of QDs was linked to the NPC-ZnO/electrode by RDNA, generating greatly amplified polarity-reversed photocurrent for signal "ON" detection of Hg2+. After specific binding of the target (aflatoxin B1, AFB1) to its aptamer, the signal probes of AIS QD-DNA nanowires were released, realizing signal "OFF" assay of AFB1. Thus, the proposed new PEC biosensor provides a versatile method for detection of dual targets and also effectively avoids both false positive and negative phenomena in the assay process, which has great practical application potential in both environmental and food analysis.

Au-quantum dot nanocluster electrochemiluminescence coupled with cycling-amplification for sensitive microRNA detection.

A novel polyamidoamine (PAMAM) dendrimer-Au nanocluster composite was synthesized, and used to fabricate a new amplified electrochemiluminescence (ECL) signal probe for sensitive detection of microRNA by multiple strand displacement amplification (SDA) strategy. The as prepared PAMAM-Au nanocluster with many amino groups could assemble a large number of quantum dots (QDs) to greatly amplify ECL of the probe. In addition, a new sliver nanocluster (NC) with excellent conductivity and many reactive carboxyl groups was prepared, and used to immobilize a large amount of capture (c1) DNA molecules on the electrode. Moreover, by using bifunctional DNA strand displacement reaction-mediated multiple cycling-amplification technique, a small number of target miRNA could induce to generate abundant DNA (t1) fragments, which was used as a linker to hybridize with c1 DNA on the electrode, and then conjugate many amplified QDs probe. Thus an amplified ECL analytical method for detecting target miRNA was designed, and highly sensitive detection of miRNA was achieved. This newly established strategy paves a new way for homogeneous microRNA detection, which hold great potential for application in early clinical diagnosis.

ß-Cyclodextrin-functionalized graphene and metal-organic framework composites for ultrasensitive electrochemical detection of chloramphenicol.

Novel ß-cyclodextrin (ß-CD)@functionalized graphene (G)/Cu-1,3,5-benzenetricarboxylic acid (BTC) composites were in situ prepared using ß-CD functionalized graphene and Cu-BTC, and a new electrochemical sensor for sensitive detection of chloramphenicol (CAP) was developed based on the composites. A series of investigations on the ß-CD@G/Cu-BTC composite material were conducted. The ß-CD functionalized graphene solution has an excellent and stable dispersion effect. The composite was further combined with metal-organic frameworks (MOFs) to overcome the disadvantages of a single material, displaying excellent conductivity and a synergistic catalytic effect on the detection of chloramphenicol; so an electrochemical sensor for CAP detection is developed. An actual sample was also detected using the proposed sensor.

Supersandwich Nanowire/Quantum Dots Sensitization Structure-Based Photoelectrochemical "Signal-On" Platform for Ultrasensitive Detection of Thrombin.

A new photoelectrochemical (PEC) "signal-on" sensing platform based on photoactive material Bi2O3-ZnO and CdS quantum dots (QDs) sensitizer was fabricated for ultrasensitive determination of thrombin by constructing supersandwich nanowires. The CdS/ZnO/Bi2O3 sensitization structure with excellent energy level arrangement remarkably improved photoelectric conversion efficiency because of the efficient separation of the electron-hole. Moreover, the DNA supersandwich nanowire is ingeniously synthesized in one step by simple dislocation hybridization, which could carry a large amount of sensitized material CdS QDs. More importantly, with Exonuclease III (Exo III)-assisted multiple amplification, the proposed "signal-on" platform demonstrated a detection range of 10 fM to 1 µM with the detection limit of 1.41 fM for thrombin. Impressively, the PEC platform can successfully detect human serum samples with good accuracy. Above all, the CdS/ZnO/Bi2O3 sensitization photoelectric biosensing platform by using DNA nanowire in combination with Exo III-multiple amplification opens new sensitized amplification paths for supersensitive biosensing and bioanalysis.

A versatile dendritical amplification photoelectric biosensing platform based on Bi2S3 nanorods and a perylene-based polymer for signal "on" and "off" double detection of DNA.

A novel versatile dendritical amplification photoelectric (PEC) biosensing platform using Bi2S3 nanorods and perylene-based polymer (PTC-NH2) as double signal probes is proposed for the detection of trace target DNA. Bi2S3 nanorods as efficient photoactive materials were firstly immobilized on the Au nanoparticle (NP) modified electrode and generated a high PEC signal. Exonuclease III (Exo III)-assisted target recycling generated a large number of DNA product chains (PC), PC hybridized with hairpin DNA (H1) on AuNPs/Bi2S3/ITO, and then triggered rolling circle amplification (RCA) and the hybridization chain reaction (HCR) to form the dendritic structure with abundant DNA duplexes. After large amounts of Mn(iii) meso-tetra(N-methyi-4-pyridyl)porphine pentachloride (MnPP) were embedded in the dendritic structure, they efficiently quenched the PEC signal, realizing the "signal off" detection of the target. In addition, the dendritic structure was also formed on AuNPs/ITO, and large amounts of PTC-NH2 molecules as the PEC probe were inserted into the dendritic structure, achieving a highly enhanced PEC current for the "signal on" detection of the target. This biosensing platform with double signals exhibits good analytical performance with wide linear ranges. This study develops a new DNA nanostructure-amplified versatile PEC sensing platform for bioanalysis, with promising potential for application in gene therapy and clinical analysis.

A dendritically amplified fluorescent signal probe on SiO2 microspheres for the ultrasensitive detection of mercury ions.

In this work, a new kind of dendritically amplified fluorescent signal probe on SiO2 microspheres was controllably fabricated by the terminal deoxynucleotidyl transferase (TdT)-catalyzed incorporation of nucleotides combined with bio-barcode (BBC) amplification for the ultrasensitive detection of Hg2+. A thymine T-Hg2+-T hairpin structure was first formed and further initiated the strand displacement amplification (SDA) reaction, generating a mimic target (MT). MT hybridized with a capture probe 1 (C1) on SiO2 microspheres, and the 3'-hydroxyl (OH) termini of MT initiated TdT-based DNA extension, producing abundant poly-guanine sequences (G1). Then, G1 hybridized with a capture probe 2 (C2) with abundant cytosine (C) species to assemble multiple C2/reporter probe-AuNPs onto the SiO2 microspheres. The reporter DNA further initiated TdT-based extension with a poly-T sequence (T1) to link large numbers of signal probes, which generated a very high fluorescence signal for the ultrasensitive detection of target Hg2+. This TdT-based signal amplification method coupled with SDA exhibits extraordinary sensitivity for Hg2+ assay with a limit down to 1.0 aM. The proposed highly sensitive fluorescence strategy holds great potential for detecting targets in environmental and biological fields.

Click chemistry reaction-triggered DNA walker amplification coupled with hyperbranched DNA nanostructure for versatile fluorescence detection and drug delivery to cancer cells.

A new DNA hyperbranched hybridization chain reaction (HB-HCR)-amplified fluorescence platform combined with DNA walker was developed for versatile detection of Cu2+, adenosine triphosphate (ATP), and drug delivery to cancer cells. A novel click chemistry reaction-triggered DNA walking machine on magnetic beads (MBs) is introduced for the first time to convert target Cu2+ to lots of DNA S3 products. With the help of DNA S3 and H1 on the amino functionalized SiO2 microsphere, HB-HCR between super hairpin DNA (SH DNA), H3-DNA, and LT-DNA was initiated to assemble a novel dendritic DNA structure with numerous fluorescent Cy5, achieving enormously amplified signal for ultrasensitive detection of Cu2+. Furthermore, this contains large amounts of double-stranded DNA with plentiful GC bases, which can provide many loading sites for chemotherapeutic drug doxorubicin (Dox). The specific binding of ATP to aptamer in the dendritic DNA structure allows for release of Dox, leading to activation of Dox fluorescence for ATP assay. More importantly, this dendritic DNA nanostructure-loaded Dox enters into tumor cells by endocytosis, and then interacts with endogenous ATP, releasing Dox for efficient treatment of cancer cells. Taking advantages of these multiple amplification of HB-HCR on SiO2 microsphere, click chemistry reaction, DNA walking, and release of Dox, this method enables ultrasensitive detection of Cu2+ and ATP as low as 0.1 fM and 1.0 aM, respectively, which can be widely used for accurate detection of biomolecules in clinical diagnosis and biomedical applications. This dendritic DNA nanostructure provided an effective tool for designing smart nanodevices. Graphical abstract.

Versatile Electrochemiluminescence and Electrochemical "On-Off" Assays of Methyltransferases and Aflatoxin B1 Based on a Novel Multifunctional DNA Nanotube.

Herein, a new multifunctional DNA nanotube (DNANT) was self-assembled and used to load Ru(phen)32+ and methylene blue (MB) as amplified signal probes for versatile electrochemiluminescence (ECL) and electrochemical (EC) "on-off" assays of Dam methylase (MTase) and aflatoxin B1 (AFB1). The DNA nanotube as a carrier could immobilize numerous MB or Ru(phen)32+ species in the double-stranded DNA (dsDNA) to significantly amplify signals, which enabled highly sensitive ECL and electrochemical detection of dual targets. The target Dam MTase first catalyzed the methylation of hairpin DNA (H1), and then the methylated DNA was cleaved by endonuclease DpnI to expose a single-strand DNA. After the Ru(phen)32+-DNANT or MB-DNANT signal probes were assembled to the electrode by hybridization, remarkable "signal on" states for amplified ECL or EC assays of MTase were obtained. Furthermore, in the presence of the target AFB1, the structure of DNANTs collapsed due to the specific binding of AFB1 to aptamer S2 in NTs, which led to the release of signal probes (Ru(phen)32+ or MB) from the electrode to achieve "signal off" state for dual detection of AFB1. Taking advantage of the multifunctional DNANT amplification signal probes, the versatile biosensors showed good analytical performance with very wide linear ranges (0.001-100 U mL-1 and 0.0001-100 ng mL-1 for MTase and AFB1 assay by DPV) and lower detection limits (2.1 × 10-4 U mL-1 and 0.018 pg mL-1 for MTase and AFB1 by DPV). This is the first time that ECL and EC "on-off" methods have been achieved separately for dual target assays, which opens a new avenue of DNANT-based signal amplification strategyies for the versatile design of biosensors in various biological detections.

Versatile Electrochemiluminescence and Photoelectrochemical Detection of Glutathione Using Mn2+ Substitute Target by DNA-Walker-Induced Allosteric Switch and Signal Amplification.

Glutathione (GSH) serves vital functions in biological systems and associates with various human diseases. In this work, a versatile electrochemiluminence (ECL) and a photoelectrochemical (PEC) "signal on" biosensing platform were developed for a sensitive assay of GSH by a Mn2+-powered DNAzyme amplification strategy combined with DNA-walker-triggered allosteric conversion. First, MnO2 nanosheets were reduced to Mn2+ by GSH; then, Mn2+ as a substitute target triggered DNAzyme-assisted cleavage-cycling amplification to generate numerous DNA output (s3). Meanwhile, the DNA molecular machine was introduced to bridge signal probes for versatile biosensing, which included hairpin DNA as a track and an arm as a walker. The presence of DNA output (s3) activated the swing arm to hybridize with hairpin DNA and then cut it by Nt.BbvCI, which initiated autonomous walking of the arm for forming a large number of streptavidin (SA) aptamers. Thus, a large number of CdS:Mn-SA tags as versatile signal probes was linked to the electrode by specific SA-aptamer binding, generating highly enhanced ECL and PEC signals for sensitive detection of the target. The present biosensing system take advantage of metal ion-based DNAzyme amplification, a DNA walker machine, multi-signals of QDs, and specificity of aptamers, which can provide a universal and efficient biosensing method for detecting various targets. The designed strategy demonstrated good performance for a GSH assay in human serum samples, showing more promising applications than other reported methods.

Multifunctional DNA nanocage with CdTe quantum dots for fluorescence detection of human 8-oxoG DNA glycosylase 1 and doxorubicin delivery to cancer cells.

A multifunctional DNA nanocage containing CdTe quantum dots (QDs) was prepared. It was applied to the fluorometric detection of human 8-oxoG DNA glycosylase 1 (hOGG1) by exonuclease-assisted cycling amplification technique. When loaded with the cancer drug doxorubicin (Dox), the nanocage is also a versatile probe for fluorescence imaging of cancer cells, and drug delivery to them. The presence of hOGG1 leads to the division of DNA HP1 (containing 8-oxo-dG) and formation of DNA fragments 1 and 2. Then, HP2 is added to hybridize with DNA 1 and produced lots of trigger DNA (containing nucleolin aptamer) by Exo III-aided cycling amplification. The DNA nanocage was fabricated by linking the trigger DNA to multiple specific DNA strands, and the fluorescent CdTe QDs were further conjugated to the DNA nanocage for sensitive detection of hOGG1 activity. After Dox is incorporated into the DNA nanocage, the fluorescence of Dox is turned off. Once the DNA nanocage enters the MCF-7 cells, the Dox is released and its fluorescence (measured at excitation/emission wavelengths of 480/560 nm) is turned on. The DNA nanocage containing fluorescent QDs and Dox was successfully applied to the fluorometric detection of hOGG1, fluorescence imaging, and therapy of cancer cells, which has great promise in clinical application and treatment of cancer. Graphical abstract A multifunctional DNA nanocage containing CdTe quantum dots and acting as a signalling probe was prepared. It was applied to fluorometric determination of human 8-oxoG DNA glycosylase 1 using cycling amplification technique. It also enables drug delivery to cancer cells if loaded with doxorubicin.

Highly intense fluorescence of novel carbon nanocrystals combined with a DNAzyme-assisted autocatalytic multiple amplification strategy for sensitive detection of thrombin.

In this work, novel water-soluble carbon nanocrystals (CNCs) with excellent fluorescence were prepared, and successfully applied to sensitive fluorescence detection of thrombin by using an enzyme-assisted autocatalytic DNA recycling amplification strategy.

Autocatalytic amplified detection of DNA based on a CdSe quantum dot/folic acid electrochemiluminescence energy transfer system.

In this work, electrochemiluminescence energy transfer (ECL-ET) from CdSe quantum dots (QDs) to folic acid is reported for the first time and applied for amplified detection of DNA by using a novel DNAzyme-mediated autocatalytic system.

A multi-modal biosensing platform based on Ag-ZnIn2S4@Ag-Pt nanosignal probe-sensitized UiO-66 for ultra-sensitive detection of penicillin.

We designed a multi-modal biosensing platform for versatile detection of penicillin based on a unique Ag-ZnIn2S4@Ag-Pt signal probe-sensitized UiO-66 metal-organic framework. Firstly, a large number of Ag-ZnIn2S4 quantum dots (AZIS QDs) were attached to Ag-Pt NPs, preparing a new multi-signal probe AZIS QDs@Ag-Pt NPs with excellent photoelectrochemistry (PEC), electrochemiluminescence (ECL), and fluorescence (FL) signals. Moreover, the AZIS QDs@Ag-Pt NPs signal probe can well match the energy level of UiO-66 metal-organic framework (MOF) with good photoelectric property, which can reverse the PEC current of UiO-66 to reduce false positives in detection. When penicillin was present, it bound to its aptamer to release the multifunctional signal probes, which can generate PEC, ECL, and PL signals, thus realizing ultrasensitive detection of penicillin by multi-signals. This work creates a novel three-signal QDs probe, which makes a great contribution to multi-mode photoelectric sensing analysis. The LOD of this work (3.48 fg·mL-1) was much lower than the MRLs (Maximum Residue Levels) established by the EU (4 ng·mL-1). The newly developed multi-mode biosensor has good practical application values in various biological detection, food assay, and early disease diagnosis.