CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Yuqing Zhu,Xiaohe Zheng,Rui Zhu,Hongrui Zhao,Hongli Zhai,Feiyang Qian,Tenghua Zhang,Zihui Xie,Silan Liu,Bowen Jiang,Yan Sheng,Jiaming Hu
Detection of multiple biomarkers for accurate diagnosis of disease is highly desirable but remains challenging. Here, we developed a versatile diagnostic biosensor (SMARTLOCK) through the unique combination of DNA tetrahedron, nonlinear HCR and CRISPR-Cas12a system for simultaneous detection of multiple nucleic acids, small molecules, proteins and different types of combinations. Two DNA tetrahedrons are assembled into a functional dumbbell lock, which was unlocked by the target molecules, thereby triggering a two-stage signal amplification of nonlinear HCR and CRISPR-Cas12a to generate powerful fluorescence signals. The capability of multi-target simultaneous detection of SMARTLOCK is demonstrated in the detection of miR-141, miR-375, miR-21, ATP, cortisol, insulin and their combinations. SMARTLOCK could selectively (specificity = 93.3%) and sensitively (sensitivity = 90%) distinguish early-stage prostate cancer (PCa) patients (n = 10) from healthy donors (n = 30). Measurement of two PCa-related RNAs (miR-141 and miR-375) shows the potential of SMARTLOCK to be a highly accurate and low-cost tool for the screening, diagnosis and prognosis of various diseases.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Jingyi Cai,Junping Ma,Yuan Dang,Shuangli Chen,Jieli Tang,Sha Yu,Yuanzhen Zhou
Antibiotics residue pollution in food and environmental matrices has posed a serious threat to global public health. It is an urgent demand in developing highly sensitive methods for the detection of low-abundance antibiotics in real samples. Herein, we established a magnetic DNA walker-engineered electrochemical sensor by taking advantages of the distinct recognition capability of aptamer and the excellent signal amplification performance of magnetic DNA walker for the accurate detection of kanamycin (Kana). The aptamer can specifically recognize Kana, while the magnetic DNA walker can not only amplify the target signal through the cascade displacement reaction, but also effectively reduce background interference via the magnetic separation, thus ensuring the sensitivity and accuracy of Kana detection in complex samples. The proposed electrochemical sensing method possesses a good linear relationship in the range of 10 fM −1 μM, and the limit of detection is as low as 0.02 fM. Moreover, the excellent selectivity allows this sensor has the ability to specifically identify the Kana from other antibiotics and even in the milk and tap water.
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ACS Sensors
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2019
·
IF 6.944
Qiong Hu,Jinming Kong,Dongxue Han,Li Niu,Xueji Zhang
Sensitive and selective sensing of biological molecules is fundamental to disease diagnosis and infectious disease surveillance. Herein, an ultrasensitive and highly selective electrochemical DNA biosensor is described by exploiting the electrochemically controlled reversible addition–fragmentation chain-transfer (eRAFT) polymerization as a signal amplification strategy and the peptide nucleic acid (PNA) probes as the recognition elements. Specifically, the PNA probes with a thiol at their 5′-terminals are anchored to a gold electrode surface (via gold–sulfur self-assembly) for sequence-specific recognition of target DNA (tDNA) fragments, of which the phosphate sites serve as the anchorages for the targeted labeling (via the well-established phosphate–Zr4+–carboxylate chemistry) of the carboxyl-group-containing chain-transfer agents (CTAs) for the succedent eRAFT polymerization, wherein the initiating radicals are generated through electrochemical reduction of aryl diazonium salts under a potentiostatic condition. In the presence of ferrocenylmethyl methacrylate (FcCH═CH2) as the monomer, the grafting of polymer chains from the CTA-anchored sites as a result of the eRAFT polymerization brings numerous electroactive Fc tags to the electrode surface, outputting a high electrochemical sensing signal even in the presence of trace amounts of tDNA fragments. Under the optimized conditions, the linear range of the described electrochemical DNA biosensor spans from 10 aM to 10 pM (R2 = 0.998), with an attomolar detection limit (4.1 aM) being achieved. Moreover, the described electrochemical DNA biosensor is highly selective and applicable to the sensing of tDNA fragments in complex serum samples. Given its high efficiency, easy operation, and low cost, this biosensor shows great promise in real applications.
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ACS Sensors
·
2019
·
IF 6.944
Xiaoqing Zhang,Ye Feng,Shaoyun Duan,Lingling Su,Jialin Zhang,Fengjiao He
The accurate and rapid detection of Mycobacterium tuberculosis (M. tuberculosis) is essential for the effective treatment of tuberculosis. In this article, we propose an electrochemical sensor to detect M. tuberculosis reference strain H37Rv. The sensor contains an H37Rv aptamer and oligonucleotides modified with gold nanoparticles (AuNPs–DNA). An H37Rv aptamer screened by our laboratory was used as the recognition probe. The change in frequency shift mediated by AuNPs–DNA in the presence of H37Rv was detected using a multichannel series piezoelectric quartz crystal (MSPQC) system. Three oligonucleotides modified with gold nanoparticles were designed. These oligonucleotides contained 12, 12, and 13 bases that hybridized with the 37-nt H37Rv aptamer. H37Rv aptamer was immobilized on the gold electrode surface by Au–S bonds. A conductive-layer was then formed by sequential hybridization of the aptamer with the three designed AuNPs–DNAs. When H37Rv was present, it specifically bound to the aptamer, resulting in the detachment of AuNPs–DNA from the electrode. The conductive layer was thereby replaced by a nonconductive complex of aptamer and bacteria. These changes were monitored by the MSPQC system. The proposed sensor is rapid, specific and sensitive, the detection time was 2 h. The detection limit was 100 cfu/mL. This sensor would be of great benefit for the early clinical diagnosis of tuberculosis.
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Journal of Materials Chemistry B
·
2019
·Vol. 7
·期 11
·1926-1932
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IF 5.047
Fanyu Meng,Hua Chai,Xiaoyi Ma,Yuguo Tang,Peng Miao
Telomerase catalyzes the elongation of telomeres, which is closely associated with tumorigenesis. Therefore, development of reliable and convenient methods for telomerase activity analysis is critical for clinical diagnosis of cancers. However, most of the current probes for intracellular telomerase activity assay suffer from inevitable false-positive interferences. In this study, we have proposed a novel fluorescence resonance energy transfer (FRET)-based strategy for ultrasensitive monitoring intracellular telomerase activity with an amplification-free procedure. DNA nanoprobes constructed using a DNA tetrahedron and Flare DNA are designed to circumvent the problem of false-positive interference. Generally, telomerase catalyzes DNA extension and changes the configuration of the DNA nanoprobe, which finally leads to the increase of the distance between two labelled fluorophores. Based on the notably decreased FRET efficiency, a simple ratiometric sensor is established for the detection of telomerase activity at the single-cell level, which is much suitable for clinical applications. In addition, this method can be further applied in the detection of telomerase inhibitors, which is important for anti-cancer drug discovery.
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ANALYTICAL SCIENCES
·
2018
·Vol. 34
·期 2
·149-153
·
IF 1.355
Xiao Fang ZHANG,Hong Mei XU,Lei HAN,Nian Bing LI,Hong Qun LUO
The detection of disease-related DNA is of great significance for early and accurate diagnosis and therapy. In this work, we successfully achieved the sensitive detection of target DNA based on a thioflavin T (ThT)-induced G-quadruplex fluorescent biosensor. ThT, a water-soluble fluorescent dye, can induce G-rich sequences to form G-quadruplexes and obtain an obviously enhanced fluorescence. In this work, it was employed to construct a biosensor for the detection of HIV. When the target HIV existed, the hairpin DNA probes would be opened in succession and release the completely exposed G-rich sequence to combine with ThT. The simple and rapid biosensor performed satisfactory selectivity; it also exhibited sensitivity with a detection limit of 2.4 nM. With good performance in human serum, we believe that this optical biosensor has the potential to be applied to the practical detection of target DNA.
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Nanoscale
·
2018
·Vol. 10
·期 35
·16508-16520
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IF 7.233
Ganglin Wang,Zhi Li,Xucheng Luo,Renye Yue,Yi Shen,Nan Ma
In situ monitoring of the photothermal (PT) effect at the cellular level is of great importance in the photothermal (PT) treatment of cancer. Herein, we report a class of DNA-templated gold nanoparticle (GNP)–quantum dot (QD) complexes (GQC) for PT sensing in solution and in cancer cells in vitro. Specifically, the QD photoluminescence (PL) could be activated at elevated temperature with a wide thermo-responsive range between 45 °C and 70 °C, which fits the temperature threshold for effective cancer cell ablation. The general applicability of GQC for intracellular PT sensing is explored using three types of PT agents (gold nanorods (GNRs), gold nanostars (GNSs), and Prussian blue nanoparticles (PBNPs)) with various PT performances. We show that the intracellular QD PL is gradually activated with increasing near-infrared (NIR) irradiation time, providing a good correlation with the surrounding medium temperature for PT sensing. Moreover, we demonstrate that the GQC sensor could be used for specific photothermal labeling and imaging of cancer cells. The QD PL signal is retained in the cells post-treatment, thereby potentially enabling persistent photothermal labeling of cancer cells for post-treatment cell tracking and imaging-guided therapy evaluation.
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BIOCHEMISTRY
·
2018
·
IF 2.997
Qianwei Zhao,Wen Yang,Tong Qin,Zhen Huang
RNA is a key player in the cellular central dogma, including RNA transcription and protein synthesis. However, it is unknown whether RNA can directly interfere with DNA synthesis. Recently, we have found in vitro that while binding to DNA polymerase nonspecifically, RNA can transform DNA polymerase to display a moonlighting activity, dNTP phosphatase, in turn interfering with DNA synthesis. This phosphatase activity removes the γ-phosphate from dNTPs (generating dNDPs) and subsequently removes the β-phosphate from the formed dNDPs (generating dNMPs), confirmed by the noncleavable α,β-CH2-dGTP and β,γ-CH2-dGTP analogues. We also found that dGTP is the best substrate for the phosphatase, and the dNTP phosphatase activity is sensitive to the reaction medium. In addition, we have revealed that RNA can tune the activity of closely related proteins and give rise to new catalytic functions with subtle differences. Moreover, we have demonstrated in vitro that at the lower dNTP level, this phosphatase can directly inhibit DNA synthesis by dNTP depletion, though the phosphatase activity is 690-fold slower than the polymerase activity. Our observation in vitro suggests a plausible strategy for RNA to directly interfere with DNA polymerase and DNA synthesis in vivo.
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Royal Society Open Science
·
2018
·Vol. 5
·期 8
·
IF 2.504
Yuting Yan,Yanwei Cao,Chunsheng Xiao,Yang Li,Xiaoxuan Xiang,Xinhua Guo
Herein, the DNA strands containing 5′-(CGA)n and consecutive guanines are used to construct supramolecular DNA nanostructures that are size-controlled by pH values. Additionally, the introduction of thymine linkers within DNA nanostructures is necessary to maintain the stability of long-sized nanostructures. This work also demonstrates a method for accurately building DNA nanostructures.
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ANALYTICAL CHEMISTRY
·
2018
·
IF 6.042
Qiong Hu,Dongxue Han,Shiyu Gan,Yu Bao,Li Niu
Sensitive detection of biomolecules is integral for biomarker screening and early diagnosis. Herein, surface-initiated reversible-addition–fragmentation-chain-transfer (SI-RAFT) polymerization is exploited as a novel amplification strategy for highly sensitive electrochemical biosensing of DNA. Briefly, thiol-terminated peptide nucleic acid (PNA) probes are first self-assembled onto a gold electrode for the specific capture of target-DNA fragments; the carboxyl-group-containing dithiobenzoate 4-cyano-4-(phenylcarbonothioylthio)pentanoic acid (CPAD) is then tethered to the hybridized PNA–DNA heteroduplexes by means of the well-established carboxylate–Zr4+–phosphate chemistry and serves as the chain-transfer agent (CTAs) for subsequent SI-RAFT polymerization, which is thermally initiated in the presence of 2,2′-azobis[2-(2-imidazolin-2-yl)propane] dihydrochloride (VA-044) as the free-radical initiator and ferrocenylmethyl methacrylate (FcMMA) as the monomer. Through SI-RAFT polymerization, one target-DNA fragment can be labeled by a large number of electroactive Fc tags, giving rise to significant amplification of the electrochemical signal. The SI-RAFT-polymerization-based strategy does not involve the use of natural enzymes or complex nanomaterials, offering the benefits of low cost and easy operation. Under optimal conditions, the electrochemical signal is linearly related to the logarithm of the concentration of target DNA over the range from 10 aM to 10 pM (R2 = 0.997), with a detection limit down to 3.2 aM, which is much lower than those of other amplification-by-polymerization-based methods. By virtue of its easy operation, low cost, and high efficiency, the SI-RAFT-polymerization-based amplification strategy is believed to have great application prospects in the sensitive detection of biomolecules.
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NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 22
·18102-18108
·
IF 3.201
Yihan Ma,Xiaoyan Zhang,Yinjia Cheng,Xiaosui Chen,Yong Li,Aiqing Zhang
Designing and constructing favorable water-dispersible fullerenes and their derivatives are of huge importance for biological applications addressing DNA-cleavage and photodynamic therapy (PDT). In the present work, a mild, green and facile synthetic approach for the preparation of C60 nanoparticles was developed for the first time via the combination of mussel-inspired chemistry and the Michael addition reaction. The resultant C60–PDA–PEI nanoparticles were characterized by transmission electron microscopy (TEM), dynamic laser scattering (DLS), Fourier-transform infrared spectroscopy (FT-IR), Raman spectra, X-ray photoelectron spectra (XPS) and thermogravimetric analysis (TGA), demonstrating that the above two-step strategy allows easy access to the preparation of highly water-dispersible fullerene derivatives. Benefiting from their unique nanostructure, the versatile C60–PDA–PEI nanoparticles display a uniform hydrodynamic size of 160 nm in water and efficient 1O2 generation under irradiation. Furthermore, the good ability of cleaving DNA under visible light at a mass concentration of 62.5 ng μL−1 gives them high potential as PDT agents. The universal approach described in this work is capable of introducing many other functional molecules onto PDA-modified fullerenes, thus extending the possible applications of fullerene-based species in many fields of biotechnology and pharmaceutical chemistry.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 7
·1-13
·
IF 5.3
Zhao Tangtang,Xiao Ruilin,Li Yueqi,Ren Jierong,Niu Liyun,Chang Bingmei
With their regulated Boolean logic operations in vitro and in vivo, DNA logic circuits have shown great promise for target recognition and disease diagnosis. However, significant obstacles must be overcome to improve their operational efficiency and broaden their range of applications. In this study, we propose an Exo III-powered closed-loop DNA circuit (ECDC) architecture that integrates four highly efficient AND logic gates. The ECDC utilizes Exo III as the sole enzyme-activated actuator, simplifying the circuit design and ensuring optimal performance. Moreover, the use of Exo III enables a self-feedback (autocatalytic) mechanism in the dynamic switching between AND logic gates within this circulating logic circuit. After validating the signal flow and examining the impact of each AND logic gate on the regulation of the circuit, we demonstrate the intelligent determination of miR-21 using the carefully designed ECDC architecture in vitro. The proposed ECDC exhibits a linear detection range for miR-21 from 0 to 300 nM, with a limit of detection (LOD) of approximately 0.01 nM, surpassing most reported methods. It also shows excellent selectivity for miR-21 detection and holds potential for identifying and imaging live cancer cells. This study presents a practical and efficient strategy for monitoring various nucleic acid-based biomarkers in vitro and in vivo through specific sequence modifications, offering significant potential for early cancer diagnosis, bioanalysis, and prognostic clinical applications. Graphical abstract
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危险品化学品经营许可证（带存储）