JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Hao Wu,Jun Wu,Hongyong Wang,Yaling Liu,Guoqing Han,Pei Zou
Malathion is one of the most commonly used organophosphorus pesticides that can cause serious harm to the ecological environment and human health. Herein, we demonstrated a label-free chemiluminescent aptasensor for the sensitive detection of malathion based on exonuclease-assisted dual signal amplification and G-quadruplex/hemin DNAzyme. Upon the addition of malathion, the aptamer probe specifically bound to the target to form a complex malathion-S3, leaving a duplex S1-S2. The complex malathion-S3 was digested by exonuclease I and the target was released. The released target was recycled to perform exonuclease I-assisted signal amplification. Furthermore, after treatment with exonuclease III, the duplex S1-S2 was converted into the secondary target ST. The secondary target ST interacted with the hairpin H1 to form a complex H1-ST, which was further digested by exonuclease III and released the secondary target. The released secondary target was recycled to perform exonuclease III-assisted signal amplification. After complete amplification, large numbers of G-quadruplex/hemin DNAzymes were generated. Under the optimal experimental conditions, the prepared aptasensor showed an excellent linear response to malathion with a detection limit of 0.47 pM. The relative standard deviations were in the range of 4.2–6.9%. Moreover, the aptasensor was successfully applied to detect malathion in spiked food and traditional Chinese medicine samples.
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MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 5
·1-9
·
IF 6.232
Cao Chen,Liu Jinquan,Tang Shuangyang,Dai Zhongran,Xiao Fubing,Rang Weiqing,Liu Ling,Chen Tuo,Yuan Yali,Li Le
A superior electrochemical biosensor was designed for the determination of UO 2 2+ in aqueous solution by integration of DNAzyme and DNA-modified gold nanoparticle (DNA-AuNP) network structure. Key features of this method include UO 2 2+ inducing the cleavage of the DNAzyme and signal amplification of DNA-AuNP network structure. In this electrochemical method, the DNA-AuNP network structure can be effectively modified on the surface of gold electrode and then employed as an ideal signal amplification unit to generate amplified electrochemical response by inserting a large amount of electrochemically active indicator methylene blue (MB). In the presence of UO 2 2+ , the specific sites on DNA-AuNP network structure can be cleaved by UO 2 2+ , releasing the DNA-AuNP network structure with detectable reduction of electrochemical response intensity. The electrochemical response intensity is related to the concentration of UO 2 2+ . The logarithm of electrochemical response intensity and UO 2 2+ concentration showed a wide linear range of 10~100 pM, and the detection limit reached 8.1 pM (S/ N = 3). This method is successfully used for determination of UO 2 2+ in water samples.
Fabricated DNAzyme network structure for enhanced electrical signal. Numerical experiments show that the current signal decreases as the concentration of UO 2 2+ increases. It can be seen that the biosensors could be used to detect UO 2 2+ in aqueous solution effectively.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Yuanling Sun,Rui Han,Yuxue Dai,Xiaodong Zhu,Hao Liu,Dandan Gao,Chuannan Luo,Xueying Wang,Qin Wei
In our work, a highly selective and sensitive streptomycin (STR) chemiluminescence (CL) sensor was successfully prepared based on aptamer and G-quadruplex DNAzyme (G-DNAzyme) modified three-dimensional graphene composite. Initially, β-cyclodextrins and ionic liquids functionalized graphene oxide aerogel (β-CD/ [email protected] ) was successfully prepared and characterized, in which graphene oxide aerogel (GOGA) was used as a skeleton material and provided large specific surface area, β-CD rich in hydroxyl groups and IL containing lots of stable ions increased the biocompatibility and stability of the composite, respectively. Then, tetracycline aptamer (S-Apt) and G-DNAzyme was immobilized on the surface of β-CD/ [email protected] , consecutively. Finally, G-DNAzyme/S-Apt/β-CD/ [email protected] was used to construct the CL sensor for STR detection. S-Apt with specific recognition ability to its target and G-DNAzyme as a catalyst of luminol-H 2 O 2 CL system improved the selectivity and sensitivity of the sensor, respectively. When STR existed, G-DNAzyme was released from the surface of S-Apt/β-CD/ [email protected] due to the specific recognition and binding ability between STR and S-Apt, catalyzing the CL reaction. The CL sensor showed the linear range of 1.4 × 10 −12 to 2.8 × 10 −9 mol/L and detection limit of 9.2 × 10 -14 mol/L (3 δ ). It was successfully used for STR detection in cucumber and milk samples.
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ANALYST
·
2019
·Vol. 144
·期 17
·5098-5107
·
IF 4.019
Shengfeng Wang,Jinsong Ding,Wenhu Zhou
Simultaneous detection and regulation of tumor-related genes presents a promising strategy for early diagnosis and treatment of cancer, but achieving this has been a huge challenge for both chemical and biomedical communities. Towards this objective, we have devised a novel aptamer-tethered, DNAzyme-embedded molecular beacon (MB) for multiple functions in cancer cells. In this design, a tumor targeting aptamer was employed to specifically deliver the sensor into cancer cells for target gene detection, and an RNA-cleaving DNAzyme was embedded to realize gene regulation. Both aptamer-tethering and DNAzyme-embedding had little influence on the sensor performance, with a detection limit of ∼2 nM and high specificity. After delivering into tumor cells, our device could monitor the tumor-related genes by producing detectable fluorescence signals, and regulate the gene expression at both mRNA and protein levels as evidenced by the RT-PCR and western blot analyses. This study provides a simple and efficient strategy to rationally combine various functional nucleic acids for multi-functional applications in living cells, which hold great potential for cancer diagnosis and therapy.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2018
·Vol. 410
·期 17
·4227-4234
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IF 3.307
Liu Hongwen,Chen Yating,Song Chunli,Tian Gang,Li Shiya,Yang Guiying,Lv Changyin
Radioactive radon decays into a stable daughter product, 210 Pb, which was used as the detection target to determine the radon radiation dose in a new technique. Pb 2+ triggers DNAzyme to cleave a molecular beacon (MB), resulting in the stem–loop structure opening and forming two single DNA strands (ssDNA). The ssDNA binds to unmodified gold nanoparticles and effectively prevents their aggregation in a salt solution. The detached enzyme strands continue to complement the remaining MB to amplify the response signal. The method proposed in this study exhibited a good linear relationship for Pb 2+ and radon concentrations in the range of 6.22 × 10 2 –1.02 × 10 5 Bq h/m 3 with a detection limit of 186.48 Bq h/m 3 using an ultraviolet–visible spectrometer. In practical applications, this sensitive method can avoid radioactive damage in field testing, and the detection limit meets the national standard in China. Importantly, this simple, highly sensitive strategy uses simple equipment and has a strong anti-interference ability.
Graphical abstract
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ANALYTICA CHIMICA ACTA
·
2018
·
IF 5.123
Weipeng Liu,Cuifen Gan,Weidan Chang,Aori Qileng,Hongtao Lei,Yingju Liu
Recently, mimic enzymes have obtained particular interest by their high activity, stability, and biocompatibility. In this work, by coupling copper hydroxide nanozyme and G-quadruplex/hemin DNAzyme to form a double-integrated mimic enzyme, a visual, sensitive and selective immunosensor was established to detect microcystin-LR (MC-LR). In this immunoassay , the microplates were modified with core-shell silica/nickel silicate as the substrate to capture MC-LR antigens. Then, Cu(OH) 2 nanocages with fine regulation were used as the label to capture the secondary antibody for immunoreaction and the DNA primer for propagation, followed by using hybridization chain reaction to amplify the DNA primer, thus numerous DNAzymes (G-quadruplex/hemin) can be formed on the surface of Cu(OH) 2 nanocages with the aid of hemin . Such double-integrated mimic enzyme including Cu(OH) 2 nanozymes and DNAzymes showed excellent peroxidase activity for the chromogenic reaction of 2,2′-azinobis-(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS), which realized the visual detection of MC-LR in the range from 0.007 to 75 μg/L with the detection limit of 6 ng/mL, and thus provided the probability for the portable assessment of MC-LR in real sample.
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ANALYTICAL CHEMISTRY
·
2013
·
IF 5.695
Wenjiao Zhou,Xue Gong,Yun Xiang,Ruo Yuan,Yaqin Chai
The employment of DNAzyme probes for visual biodetections has received increasing interest recently due to the simple nature of this type of assay. However, achieving high sensitivity and detecting targets beyond nucleic acids remain two major challenges in DNAzyme-based visual detections. In this work, based on a new quadratic amplification strategy, we developed a sensitive and visual detection method for cytokines by using hairpin aptamer DNAzyme probes. The target cytokine, interferon γ (IFN-γ), associates with the aptamer sequences and unfolds the hairpin structure of the probes, leading to simultaneous recycling of the target IFN-γ (assisted by Bst-polymerase) and the DNA sequences (aided by λ exonuclease) to achieve quadratic amplification. This quadratic amplification results in the generation of numerous peroxidase-mimicking DNAzymes, which cause significantly intensified color change of the probe solution for highly sensitive detection of IFN-γ by the naked eye down to 50 pM. The proposed visual sensing method shows also high selectivity toward the target IFN-γ and can be performed in homogeneous solutions with using completely unmodified, synthetic aptamer DNAzyme probes. These distinct advantages of our developed assay protocol make it a potential platform for detecting various types of biomolecules with careful probe designs.
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ANALYTICAL BIOCHEMISTRY
·
2014
·
IF 2.305
Hui Liu,Yong-Sheng Wang,Jia-Cheng Wang,Jin-Hua Xue,Bin Zhou,Hui Zhao,Shan-Du Liu,Xian Tang,Si-Han Chen,Ming-Hui Li,Jin-Xiu Cao
A highly sensitive, low-cost colorimetric aptasensor was developed for the determination of 8-hydroxy-2′-deoxyguanosine (8-OHdG) in human urine. The method is based on a conformational switching of the 8-OHdG aptamer to form a G-quadruplex structure in the presence of 8-OHdG. The resulting G-quadruplex assembles into a peroxidase-like DNAzyme with hemin , which effectively catalyzes the oxidation of 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) diammonium salt (ABTS 2− ) by H 2 O 2 to ABTS + , resulting in an increase in the absorption signal at 416 nm along with a color change of the solution. The response signals linearly correlated with the concentration of 8-OHdG, ranging from 466 pM to 247 nM with a detection limit of 141 pM. The relative standard deviation and the recovery were 1.97–3.47% ( n = 11) and 98.8–100.2%, respectively. The proposed method avoids the label and derivatization steps in common methods and allows direct analysis of the samples by the naked eye without costly instruments, which is reliable, inexpensive, and sensitive.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Xinqi Long,Qi Wu,Lu Yang,Longyingzi Xie,Lanrui Ma,Qiyang Zhao,Yongliang Cui,Yue He,Yaohai Zhang
Aptasensors for detection of ochratoxin A (OTA) have been extensively studied, but the majority of them require costly and large-scale equipment as signal readers. Herein, a photothermal aptasensor capable of portable detection of OTA through a thermometer was developed on basis of aptamer structural switching and rolling circle amplification (RCA)-enriched DNAzyme. Oligonucleotides and alkaline phosphatase (ALP) modified magnetic beads were prepared. The binding of aptamers to OTA led to the release of ALP labeled complementary DNA. After magnetic separation, ALP catalyzed the padlock dephosphorylation, inhibiting the subsequent RCA reaction. This process converted the OTA concentration into the amount of the photothermal reagent oxTMB produced from the catalytic reaction induced by RCA-enriched DNAzyme. Under the optimal conditions, the detection limit (LOD) of this aptasensor was 2.28 nM in a clean buffer, while the LOD reached 2.43 nM in 2 % grape juice. The good performance of the photothermal aptasensor makes it possible to measure OTA pollution in low resource environments.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2017
·
IF 3.012
Hai-Yan Song,Tian-Fang Kang,Meng-Fan Jiang,Jing-Jing Zhang,Shui-Yuan Cheng
A novel, simple, and versatile electrochemiluminescence (ECL) sensing platform for Pb(II) ions was developed based on DNAzyme with peroxidase-like activity to catalyze the reduction of hydrogen peroxide. Poly (diallyldimethylammonium chloride) (PDDA) with positive charge was adsorbed onto the surface of graphene oxide (GO) and then CdS quantum dots (QDs) with negative charge were enriched to the surface of GO by electrostatic interaction between CdS QDs and PDDA to prepare a composite (denoted as [email protected] ) which was immobilized on the surface of a glassy carbon electrode (GCE). When hydrogen peroxide was used as coreactant CdS QDs can produce ECL signal. G-rich DNA strand, i . e . T30695, can combine with Pb (II) ions to form a stable parallel G-quadruplex. The G-quadruplex can further combine with hemin to form DNAzyme which have catalysis towards the reduction of hydrogen peroxide causing the decrease of ECL signal. Amino-modified T30695 was attached to [email protected] composite by the reaction between the amino group of T30695 and carboxyl group of CdS QDs. The ECL signal of the biosensor was linearly dependent on the logarithm of Pb(II) concentration from 1.0 × 10 − 14 to 1.0 × 10 − 11 M with a detection limit of 9 fM. An excellent performance of ECL biosensor indicated that it is promising for Pb(II) detection in real samples.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Xiuhua Zhang,Heqin Liu,Wanrong Hong,Yumin Wang,Jin-Wen Liu,Yingfeng Qin
In this work, a novel fluorescence nanoprobe based on MnO 2 nanosheets and DNAzyme cyclic amplification was developed for label-free detection of GSH. In our design, the DNA@MnO 2 nanoprobe was facilely prepared through the adsorption of DNA probes on the surface of MnO 2 nanosheets. Importantly, MnO 2 nanosheets in the DNA@MnO 2 nanoprobe can act as the recognizer of analytical target GSH. In the presence of GSH, the DNA@MnO 2 nanoprobe are decomposed owing to redox-responsive reaction between GSH and MnO 2 nanosheets, resulting in the generation of abundant Mn 2+ and the desorption of DNA probes. Subsequently, the Mn 2+ -dependent DNAzyme recycling amplification was rapidly initiated and a large number of the blocked G-rich sequences in DNA probes was released. The G-rich sequences were efficiently folded into G-quadruplex structures, which can remarkably light up the fluorescence intensity of thioflavin T (ThT). Experimental data demonstrated that the DNA@MnO 2 nanoprobes for GSH detection have a wide linear range from 0 to 2000 µM. Moreover, this fluorescence sensing strategy was successfully applied for the detection of GSH in complex biological media with satisfying results, providing a simple, facile and cost-efficient nanoplatform for GSH-related clinical disease diagnosis.
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TALANTA
·
2026
·
IF 6.7
Hengxin Yu,Guohai Lin,Jing Jiang,Miaomiao Cai,Yue Qiao,Huo Xu
Lead ions (Pb 2+ ), as a persistent and bioaccumulative environmental toxin, pose a significant threat to public health, demanding ultrasensitive and field-deployable detection methods. Conventional sensors often struggle with a trade-off between sensitivity and stability, especially when employing hard nanomaterial enhancers like gold nanoparticles. However, the practical utility of these inorganic nanoprobes is often compromised by their susceptibility to surface passivation (biofouling) and aggregation in salt-rich or protein-rich environments. Herein, we introduce a novel concept of a soft-matter DNA nanoreactor for engineering a high-performance colorimetric biosensor. This nanoreactor is self-assembled from a single palindromic DNA strand into a DNA nanosphere (DS), creating a spatially confined microenvironment. By anchoring a Pb 2+ -specific DNAzyme system onto this platform, we developed the DS-S-Dz probe. The nanoreactor architecture dramatically enhances the catalytic efficiency of the DNAzyme through a profound spatial confinement effect, which accelerates the Pb 2+ -triggered cleavage of a substrate strand and subsequent release of a G-rich sequence. This liberated sequence then folds into a G-quadruplex/hemin DNAzyme, catalyzing a robust colorimetric reaction. This strategy effectively suppresses background noise while amplifying the target signal, achieving a remarkable limit of detection of 0.96 nM, a 50-fold improvement over the non-amplified system (48 nM) and well below the EPA safety limit (72 nM). The sensor demonstrated exceptional selectivity against a panel of interfering metal ions and proved its robustness and accuracy in complex real-world samples like tap water and milk. This work presents a paradigm shift from simple nanoparticle enhancement to the rational design of programmable DNA nanoreactors, offering a powerful and elegant platform for sensitive and reliable environmental monitoring.
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