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ANALYTICAL CHEMISTRY · 2020 · IF 6.785

Plasmonic SERS Au Nanosunflowers for Sensitive and Label-Free Diagnosis of DNA Base Damage in Stimulus-Induced Cell Apoptosis

Guohua Qi,Dandan Wang,Chuanping Li,Kongshuo Ma,Ying Zhang,Yongdong Jin

Molecular diagnosis and accurate damage analysis of complex genomic DNAs in tumor cells are crucial to the theranostics of cancers but still a huge challenge. Herein, by designed preparation of a uniform plasmonic sunflower-like assembly gold (Au) nanostructure that is capable of efficient DNA capture and providing high-density gap-plasmon “hot spots” for adequate surface-enhanced Raman spectroscopy (SERS) enhancement, we succeeded in sensitive and reliable label-free SERS detection of DNA damage in electrostimulus-induced apoptotic cancer cells at the DNA base level for the first time. The SERS results showed that the external electrostimulus (at 1.2 V, for 5 min) was almost harmless to normal healthy cells, but it caused pronounced double strand break and adenine base damage in cancer cell DNAs, which effectively destroyed the reproduction and transcription of DNAs and ultimately induced cell apoptosis. The developed sensing platform and method are promising for cell study of genetically related diseases.

CAS / MDL: 16961-25-4
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Metal–Organic Framework in Situ Post-Encapsulating DNA–Enzyme Composites on a Magnetic Carrier with High Stability and Reusability

Zixin Zhou,Zijing Gao,Hao Shen,Mengqi Li,Wenting He,Ping Su,Jiayi Song,Yi Yang

In recent years, metal–organic frameworks (MOFs) have been extensively studied as candidate enzyme immobilization platforms. However, conventional MOF–enzyme composites usually exhibit low controllability and reusability. In this study, a novel and stable strategy for enzyme immobilization was designed by use of ZIF-8 to encapsulate in situ DNA–enzyme composites on the surface of magnetic particles (MPs). The mechanism of in situ encapsulation was discussed in detail. It was found that immobilized enzymes were involved in the growth of ZIF-8, and the DNA cross-linking agents promoted the growth of ZIF-8 on the surface of MP. The thermal, chemical, and physical stabilities of horseradish peroxidase (HRP) were all significantly enhanced after in situ encapsulation. Most importantly, this strategy was proven to be a general platform that can be used to stabilize various proteins. The in situ encapsulation strategy was expanded to immobilize a cascade of enzymes, and ZIF-8@MPGOx–HRP possessed high selectivity and a wide linear range (25–500 μM) for glucose detection.

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SENSORS AND ACTUATORS B-CHEMICAL · 2020 · IF 7.1

Three-dimensional mesoporous dendritic fibrous nanosilica as a highly efficient DNA amplification platform for ultrasensitive detection of chlorpyrifos residues

Jianhui Liu,Deyu Kong,Zhen Liu,Hanbiao Liu,Jiangle Yi,Dong Tian,Fangquan Xia,Changli Zhou

In this paper, a novel amino-functionalized mesoporous dendritic fibrous nanosilica (NH 2 -DFNS) was used as DNA amplification platforms with DNA generated electrochemical signal as target conversion strategy to establish an electrochemical aptasensor for chlorpyrifos residues. The signal generation was based on the electrochemical reaction between molybdate with phosphate groups on the aptamer molecules, which greatly simplified the signal transduction and preparation steps of aptasensor, so as to improve the sensitivity of the aptasensor. The NH 2 -DFNS was prepared by a simple microemulsion method and characterized by SEM, TEM, FT-IR, BET, as well as XPS techniques. Importantly, the results showed that such a sphere-shaped nanomaterial with three-dimensional (3D) centerradial channels and hierarchical pores supported abundant DNA to amplify the DNA generated signal in the aptasensor. Furthermore, this aptasensor for detection of chlorpyrifos showed good sensitivity with a linear range of 1.0 fM∼1.0 nM, a detection limit of 0.43 fM. In addition, this sensor also possessed excellent specificity, repeatability, and stability. Moreover, this proposed electrochemical aptasensor was successfully used for the detection of chlorpyrifos residues in several practical samples.

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MICROCHIMICA ACTA · 2020 ·Vol. 187 ·期 5 ·1-9 · IF 6.232

Amplified electrochemical determination of UO22+ based on the cleavage of the DNAzyme and DNA-modified gold nanoparticle network structure

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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ELECTROCHIMICA ACTA · 2020 · IF 6.215

RNA aptamer-driven ECL biosensing for tracing histone acetylation based on nano-prism substrate and cascade DNA amplification strategy

Qingqing Zhang,Tingting Hao,Dandan Hu,Zhiyong Guo,Sui Wang,Yufang Hu

A new RNA aptamer-involved electrochemiluminescence (ECL) strategy for sensitive detection of histone acetyltransferase (HAT p300) is designed well based on coenzyme A (CoA)-initiated competitive response and advanced DNA nano-biotechnology. For the first time, this interesting analytical process is comprised of significant histone acetylation catalyzed by HAT p300, competitive replacement triggered by the specific binding of CoA and its RNA aptamer , stable scaffold guided by DNA nano-prism and typical amplification managed by hybrid chain reaction (HCR). Upon recognition of the RNA aptamer to CoA generated in acetylation, auxiliary DNA (A-DNA) which can be captured by three hanging arms of the fabricated DNA nano-prism immobilized onto Au electrode surface is released from the aptamer/A-DNA complex. Moreover, A-DNA can also open skillfully one hairpin DNA (H1), then turning into HCR process by alternating hybridization with the other hairpin DNA (H2). Abundant Ru(phen) 3 2+ molecules which have a strong interaction with dsDNA can result in a significant output. This proposed platform exhibits excellent specificity and sensitivity toward HAT p300 with a detection limit of 0.001 nM and takes on outstanding practicality and superiority, which presents a great potential for HAT p300 analysis in biomedical sciences.

CAS / MDL: 23570-43-6 9000-81-1
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Frontiers in Chemistry · 2020 · IF 3.693

A Fluorescence Resonance Energy Transfer Probe Based on DNA-Modified Upconversion and Gold Nanoparticles for Detection of Lead Ions

Wang Yue,Lv Menghua,Chen Zehan,Deng Zilong,Liu Ningtao,Fan Jianwei,Zhang Weixian

We report a new sensor for the specific detection of lead ions (Pb2+) in contaminated water based on fluorescence resonance energy transfer (FRET) between upconversion nanoparticles (UCNPs) as donors and gold nanoparticles (Au NPs) as receptors. The UCNPs modified with Pb2+ aptamers could bind to Au NPs, which were functionalized with complementary DNA through hybridization. The green fluorescence of UCNPs was quenched to a maximum rate of 80% due to the close proximity between the energy donor and the acceptor. In the presence of Pb2+, the FRET process was broken because Pb2+ induced the formation of G-quadruplexes from aptamers, resulting in unwound DNA duplexes and separated acceptors from donors. The fluorescence of UCNPs was restored, and the relative intensity had a significant linear correlation with Pb2+ concentration from 0 to 50 nM. The sensor had a detection limit as low as 4.1 nM in a buffer solution. More importantly, the sensor exhibited specific detection of Pb2+ in complex metal ions, demonstrating high selectivity in practical application. The developed FRET prober may open up a new insight into the specific detection of environmental pollution.

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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Lattice-Like DNA Tetrahedron Nanostructure as Scaffold to Locate GOx and HRP Enzymes for Highly Efficient Enzyme Cascade Reaction

Ding Wang,Yaqin Chai,Yali Yuan,Ruo Yuan

In this work, the array arrangement of cascade enzymes was implemented by alternately and equidistantly anchoring two model enzymes glucose oxidase (GOx) and horseradish peroxidase (HRP) to the vertexes of rigid DNA tetrahedron units in lattice-like nucleic acid scaffold, in which the distance between any adjacent cascade enzymes had been regulated to the optimum for obtaining high enzyme cascade catalytic efficiency. Compared to the enzyme cascade system with no-array arrangement of cascade enzymes, the proposed enzyme cascade system allowed the intermediate H2O2 produced by GOx catalyzing substrate glucose to concurrently and equidistantly diffuse toward the four adjacent HRP enzyme surfaces. In this case, the invalid diffusion effect of intermediate H2O2 between cascade enzymes could be effectively avoided, thereby promoting the enzyme cascade reaction with high catalytic efficiency. The specific catalytic efficiency (kcat/Km) of the cascade enzyme system with array arrangement had been evaluated, which exhibited catalytic efficiency about 3.6 times higher than that of the randomly arranged cascade enzyme system. As a result, this strategy provided a new avenue for constructing a highly efficient enzyme cascade system with ultimate applications in biosynthesis, bioanalysis, and biodiagnostics.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Oxidative Medicine and Cellular Longevity · 2019 · IF 4.868

Exosomal miRNA Let-7 from Menstrual Blood-Derived Endometrial Stem Cells Alleviates Pulmonary Fibrosis through Regulating Mitochondrial DNA Damage

Lifang Sun,Min Zhu,Wei Feng,Yiping Lin,Jia Yin,Juan Jin,Yunguang Wang

Idiopathic pulmonary fibrosis (IPF) is a prototype of chronic, progressive, and fibrotic lung disease with high morbidity and high mortality. Menstrual blood-derived stem cells (MenSCs) have proven to be an attractive tool for the treatment of acute lung injury and fibrosis-related diseases through immunosuppression and antifibrosis. However, whether MenSC-derived exosomes have the similar function on pulmonary fibrosis remains unclear. In the present study, exosomes secreted from MenSCs (MenSCs-Exo) were verified by transmission electron microscope (TEM), nanoparticle tracking analyzer (NTA), and western blotting. And MenSC-Exo addition significantly improved BLM-induced lung fibrosis and alveolar epithelial cell damage in mice, mainly reflected in BLM-mediated enhancement of the fibrosis score, blue collagen deposition, dry/wet gravity ratio, hydroxyproline and malondialdehyde levels, and downregulation of glutathione peroxidase, which were all robustly reversed by MenSC-Exo management. Additionally, BLM- and TGF-β1-evoked cellular reactive oxygen species (ROS), mitochondrial DNA (mtDNA) damage, and cell apoptosis were rescued by MenSCs-Exo in vivo and in vitro. Further study indicated that the MenSCs-Exo could transport miRNA Let-7 into recipient alveolar epithelial cells. Let-7 inhibitor administration significantly blocked the exosome-mediated improvement role on lung fibrosis in mice. Mechanistically, Let-7 was able to regulate the expression of lectin-like oxidized low-density lipoprotein receptor-1 (LOX1) through binding to its 3-UTR region. Forced expression of LOX1 promoted the expression of apoptosis-related protein and mtDNA damage markers via regulating NLRP3 which was also confirmed in BLM model mice under the combination therapy of the exosome and Let-7 inhibitor. Collectively, this study demonstrates that exosomal Let-7 from MenSCs remits pulmonary fibrosis through regulating ROS, mtDNA damage, and NLRP3 inflammasome activation. This provides a new approach of exocytosis on the treatment of fibrotic lung disease.

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ANALYTICAL CHEMISTRY · 2019 · IF 6.35

Separation-Free Electrogenerated Chemiluminescence Immunoassay Incorporating Target Assistant Proximity Hybridization and Dynamically Competitive Hybridization of a DNA Signal Probe

Bing Wang,Suwen Shi,Xiaolin Yang,Yue Wang,Honglan Qi,Qiang Gao,Chengxiao Zhang

A separation-free electrogenerated chemiluminescence (ECL) immunoassay for biomarkers has been developed incorporating target assistant proximity hybridization and dynamically competitive hybridization of a DNA ECL signal probe for the first time. In this work, the biomarkers of acute myocardial infarction including cardiac troponin I (cTnI), cardiac troponin T (cTnT), and myoglobin (Myo) were chosen as the model proteins while the corresponding antibody was utilized as a recognition probe and the DNA5 tagged with ruthenium complex was chosen as an ECL signal probe (DNA5-Ru1). The biosensors were fabricated by covalently coupling the capture probe DNA1 onto the surface of a glassy carbon electrode, and then, a competitor ss-DNA2 was hybridized with DNA1. When the biosensor was incubated in the solution containing a target protein, the recognition probes (DNA3-Ab1 and DNA4-Ab2), DNA5-Ru1, and the coreactant tri-n-propylamine, the target protein was bounded with two antibodies of the recognition probes and thus induced the sufficient proximity hybridization of DNA3 with DNA1, DNA4 with DNA5-Ru1, and DNA5-Ru1 with DNA1 and the unwinding of the competitor DNA2 with DNA1, and ECL measurement was performed in separation-free format. It was found that the hybridization base number and length of DNA1 and a competing hybridization of DNA5-Ru1 with DNA2 for DNA1 have important effects. The developed ECL method showed a quite low detection limit of 0.4 pg/mL for cTnI, 0.5 pg/mL for cTnT, and 0.5 ng/mL for Myo. The fabricated biosensor exhibited stability and reusability. This work demonstrated that the developed ECL immunoassay is a promising separation-free and flexible strategy for quantitation of multiple proteins using one biosensor.

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JOURNAL OF MOLECULAR STRUCTURE · 2019 · IF 2.12

Construction of six complexes from 2-(2-pyridyl)benzothiazole and polycarboxylic acids: Synthesis, crystal structures and DNA-binding properties

Yu Yang,Jiang-Yu Bian,Yu-Han Li,Hui-Chao Guan,Yan-Ru Tang,Yan-Ling Chen,Shu-Mei Yue

Six complexes including [Cd (bpt)(odc) 2 ] (1), [Ni(bpt)(odc) 2 ] (2), [Zn (bpt)(odc) 2 ] (3), [Zn (bpt)(1,4-ndc) 2 (H 2 O)] (4), [Cd (bpt)(1,4-ndc) 2 ] (5), [Cd (bpt)(Pta) 2 (H 2 O) 2 ] (6), {bpt = 2-(2 pyridyl)benzothiazole, H 2 odc = 4,4′-oxybisbenzoic acid, 1,4-H 2 ndc = naphthalene-1,4-dicarboxylic acid, Pta = terephthalic acid}, have been determined by single-crystal X-ray diffraction analysis, which shows that complexes 1–3 belong to monoclinic system with space group P2 1 /n, complex 4 and complex 6 belong to triclinic system with space group P-1, complex 5 belongs to monoclinic system with space group P2 1 /c. TD-DFT calculations for the complexes 3 was performed to explain the structures and electronic spectral properties. UV spectroscopy , fluorescence spectroscopy and viscosity were used to characterize the interaction of the CT-DNA complexes. The results indicate that complexes 1–6 have strong interaction with CT-DNA binding. All complexes exhibit an electrostatic or groove mode of binding with DNA . Furthermore, they also present that all complexes have strong ability to interact with DNA. It can effectively destroy the DNA acting on cancer cells. Therefore, we hope to provide a theoretical and scientific basis for the development of anti-cancer drugs.

CAS / MDL: 1185-53-1
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Target-Driven Cascade-Amplified Release of Loads from DNA-Gated Metal–Organic Frameworks for Electrochemical Detection of Cancer Biomarker

Ting Bao,Ruobing Fu,Wei Wen,Xiuhua Zhang,Shengfu Wang

In this paper, a label-free and stimuli-responsive electrochemical biosensing platform was fabricated based on target-driven load release from DNA-gated metal–organic frameworks (MOFs) with cascade amplification. By using MOFs (UiO-66-NH2) as a nanocarrier of electroactive molecules (methylene blue; MB) and the programmably assembled DNA acted as the gatekeeper, the biofunctionalized MOFs (MB@DNA/MOFs) were not only used as an amplified signal label but also worked as three-dimensional tracks for biosensing. In the presence of a target, the nicking endonuclease cleavage process was triggered, leading to the generation of two strands (S1 and S2). Both S1 and S2 act as stimuli to participate in the strand displacement reaction on the MB@DNA/MOFs, which caused the unlocking of the pore to release MB, resulting in the decrease of the signal. Using carcinoembryonic antigen (CEA) as a model target, the cascade-amplified biosensor presented good performance for CEA detection, ranging from 50 fg/mL to 10 ng/mL with a detection limit of 16 fg/mL. The stimuli-responsive DNA-gated MOF-based electrochemical platform exhibited three-dimensional biosensing tracks with rational utilization of the cascade amplification, providing an effective method for cancer biomarker detection.

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SENSORS AND ACTUATORS B-CHEMICAL · 2023 · IF 8.4

Tris(2-carboxyethyl)phosphine-mediated immobilization of thiolated DNA on gold nanoclusters and its application in multiplex microRNA detection

Weidong Qin,Junhua Wang,Zhanqiu Tang,Hongyuan Tian,Zhenglong Wu

Quick and efficient immobilization of DNAs on gold nanoclusters (AuNCs) has a substantial impact on nanoscale applications relative to molecular recognition and patterned assembly. We found that in the presence of tris(2-carboxyethyl)phosphine (TCEP), chemisorption of thiolated DNA on the AuNC surface could be accomplished within 1.5 h, which was dramatically shorter than the incubation time needed in the conventional thiolate exchange reactions. Based on this observation, a core-shell-satellite nanocomposite consisting of magnetic nanoparticle , silica coating, and AuNCs (Fe 3 O 4 NPs@SiO 2 @AuNCs) was fabricated, on which a fluorescent hairpin probe was anchored with the assistance of TCEP. Integrated with duplex-specific nuclease (DSN)-assisted target recycling strategy, the sensing platform could simultaneously detect microRNA-21 and microRNA-141 with detection limits of 0.020 and 0.017 pM, respectively. The feasibility of the developed immobilization approach might significantly advance the use of DNAs and AuNCs in analytical sciences and clinical research.

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