ACS Applied Materials & Interfaces
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2022
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IF 10.383
Tongtong Guo,Yuanhang Xiang,Hao Lu,Minmin Huang,Fengfei Liu,Min Fang,Jia Liu,Yujin Tang,Xinchun Li,Fan Yang
Interfacial DNA self-assembly is fundamental to solid nucleic acid biosensors, whereas how to improve the signal-to-noise ratio has always been a challenge, especially in the charge-based electrochemical DNA sensors because of the large noise from the negatively charged DNA capture probes. Here, we report a DNA framework-reversed signal-gain strategy through background-to-signal transition for ultrasensitive and highly specific electrical detection of microRNAs (miRNAs) in blood. By using a model of enzyme-catalyzed deposition of conductive molecules (polyaniline) targeting to DNA, we observed the highest signal contribution per unit area by the highly charged three-dimensional (3D) tetrahedral DNA framework probe, relative to the modest of two-dimensional (2D) polyA probe and the lowest of one-dimensional (1D) single-stranded (ss)DNA probe, suggesting the positive correlation of background DNA charge with signal enhancement. Using such an effective signal-transition design, the DNA framework-based electrochemical sensor achieves ultrasensitive miRNAs detection with sensitivity up to 0.29 fM (at least 10-fold higher than that with 1D ssDNA or 2D polyA probes) and high specificity with single-base resolution. More importantly, this high-performance sensor allows for a generalized sandwich detection of tumor-associated miRNAs in the complex matrices (multiple cell lysates and blood serum) and further distinguishes the tumor patients (e.g., breast, lung, and liver cancer) from the normal individuals. These advantages signify the promise of this miRNA sensor as a versatile tool in precision diagnosis.
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LUMINESCENCE
·
2022
·Vol. 37
·期 8
·1275-1283
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IF 2.613
Shuyun Bi,Xu Li,Zhixin Ren,Bin Yang,Yuting Wang,Fengming Zhang,Yue Yuan,Di Shao,Rui Zhao
The binding of tiamulin with calf thymus DNA was systematically investigated using multispectroscopy and molecular modelling techniques. For DNA, once tiamulin was added, viscosity ( η ) and melting temperature ( T m ) both exhibited an uptrend. The fluorescence performance of the tiamulin–DNA complex did not change with the ionic strength changes. The binding constant ( K a ) of tiamulin for single-stranded DNA (ssDNA, 1.48 × 10 4 M −1 ) was obviously higher than that for double-stranded DNA (dsDNA, 9.51 × 10 3 M −1 ) at 291 K. The helix structure became looser and the base stack force became stronger for DNA due to the presence of tiamulin as seen from circular dichroic (CD) spectra. The intercalation binding mode of tiamulin with DNA was disclosed. Molecular modelling also revealed tiamulin inserting into the base pairs with the lowest binding free energy of −18.73 kJ mol −1 using van der Waals forces as well as hydrogen bonds.
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ANALYTICAL CHEMISTRY
·
2022
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IF 8.008
Qiong Hu,Jianwen Wan,Yilin Luo,Shiqi Li,Xiaojing Cao,Wenxing Feng,Yiyi Liang,Wei Wang,Li Niu
In view of their high efficiency and cost-effectiveness, polymers are of great promise as carriers for signal tags in amplified detection. Herein, we present a polysaccharide-amplified method for the electrochemical detection of a BRCA1 breast cancer gene-derived DNA target at the femtomolar levels. Briefly, peptide nucleic acid (PNA) with a complementary sequence was tethered as the capture probe for the DNA target, to which carboxyl group-containing polysaccharides were then attached via facile phosphate-Zr(IV)-carboxylate crosslinking, followed by the decoration of polysaccharide chains with electroactive ferrocene (Fc) signal tags via affinity coupling between a cis-diol site and phenylboronic acid (PBA) group. As the polysaccharide chain contains hundreds of cis-diol sites, boronate affinity can enable the site-specific decoration of each polysaccharide chain with hundreds of Fc signal tags, efficiently transducing each target capture event into the decoration of many Fc signal tags. As polysaccharides are cheap, renewable, ubiquitous, and biodegradable natural biopolymers, the use of polysaccharides for signal amplification offers the benefits of high efficiency, cost-effectiveness, excellent biocompatibility, and environmental friendliness. The linear range of the polysaccharide-amplified method for DNA detection was demonstrated to be from 10 fM to 10 nM (R2 = 0.996), with the detection limit as low as 2.9 fM. The results show that this method can also discriminate single base mismatch with satisfactory selectivity and can be applied to DNA detection in serum samples. In view of these merits, the polysaccharide-amplified PNA-based electrochemical method holds great promise in DNA detection with satisfactory sensitivity and selectivity.
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Frontiers in Chemistry
·
2022
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IF 5.545
Fan Zhang,Changqing Mao,Siyu Cao,Runchi Zhang,Yi Guo,Guifang Chen,Chang Feng
Bio-nanomicelles based on biomaterials such as nucleic acids, peptides, glycans, and lipids have developed rapidly in the field of bioanalysis. Although DNA and peptides have unique advantages, unfortunately, there are few bio-nanomicelles integrating DNA with peptides. Here, we designed a peptide-DNA hybrid bio-nanomicelle for the activity detection of caspase-3. The detection mechanism is based on caspase-3 specific recognition and cleavage of peptide substrates, which owns high sensitivity and selectivity. Under optimal conditions, the detection of caspase-3 activity can be achieved using our designed bio-nanomicelles and the detection limit is 0.72 nM. Furthermore, the proposed method was also successfully applied for the detection of caspase-3 in cell lysate samples after apoptosis-inducing.
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高影响因子
LUMINESCENCE
·
2022
·Vol. 37
·期 11
·1964-1971
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IF 2.613
Long Bai,Tai Ye,Dongdong Zhu,Donghao Sun,Shuyi Zhang,Yujie Lu,Min Yuan,Hui Cao,Liling Hao,Xiuxiu Wu,Fengqin Yin,Fei Xu
The improper conformation of oligonucleotides on gold nanoparticle surfaces is caused by unintended base adsorption, which hinders DNA hybridization and lowers colloidal stability. In this work, we treated spherical nucleic acids with Br − , which serves as an efficient backfilling agent, to adjust the DNA conformation by displacing bases from the gold surface. To investigate the effect of DNA conformation on interfacial recognition, a kanamycin fluorescent aptasensor was constructed with bromide backfilled-treated spherical nucleic acids. In the presence of kanamycin, the anchored aptamer binds with the target and the partially complementary reporter strand is dissociated from the surface of the gold nanoparticles, resulting in the fluorescence recovery of labelled fluorophore on the reporter strand. Under optimum conditions, the apparent binding affinity of the aptasensor with bromide backfilling was 2.2-fold that without backfilled one. The proposed aptasensor exhibited a good liner relationship between the concentration of kanamycin and fluorescence intensity change in the range 200 nM to 10 μM and the limit of detection was calculated to be 71.53 nM. Moreover, this aptasensor was also successfully applied in a spiked milk sample assay and the satisfactory recoveries were obtained in the range 96.94–101.57%, which demonstrated its potential in practical applications.
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ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Xiaofen Zhao,Xiaoxiao Tian,Yuwei Wang,Linbin Li,Yan Yu,Shiqiao Zhao,Juan Zhang
Accurate analysis of HIV DNA is valuable for the diagnosis of AIDS. Herein, an ultrasensitive and specific fluorescence method was developed for HIV-1 DNA detection based on CRISPR-Cas12a-activated palindrome-catalytic hairpin assembly (CRISPR-Cas12a-PCHA). The presence of HIV-1 DNA activated the trans-cleavage activity of CRISPR-Cas12a, which could continuously digest the DNA fragment of hairpins connected to magnetic beads to expose single-stranded RNA . After magnetic separation, the exposed RNA triggered multiple PCHA reactions, generating many Y-shaped DNA structures that were self-assembled into the DNA superstructures via the hybridization of palindromic sticky ends, leading to the release of amounts of fluorescence signal. Different from the reported recently biosensing strategies of nucleic acid amplification technologies-activated CRISPR-Cas12a, CRISPR-Cas12a-PCHA endowed the strategy with unique advantages of simple sample pretreatment , direct duplex target detection, and ultrahigh sensitivity. The strategy was able to resist the interference of the complex matrix in real sample and distinguish between HIV patients and healthy persons. Thus, the method is a promising tool for ultrasensitive and specific detection of HIV-1 DNA for AIDS diagnosis.
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RSC Advances
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2022
·Vol. 12
·期 29
·18296-18300
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IF 4.036
Xiaofei Liao,Mengyan Li,Li Zou
In this work, a label-free and sensitive colorimetric sensing strategy for the detection of bleomycin (BLM) was developed on the basis of BLM-mediated activation of G-quadruplex DNAzyme via DNA strand scission. A G-quadruplex based hairpin probe (G4HP) containing the scission site (5′-GT-3′) of BLM at the loop region and guanine (G)-rich sequences at its 5′-end was employed in this protocol. In the presence of BLM, it may cleave the 5′-GT-3′ site of the hairpin probe with Fe(II) as a cofactor, releasing the G-tetrads DNA fragment, which may further bind hemin to form a catalytic G-quadruplex-hemin DNAzyme. The resultant G-quadruplex DNAzyme has notable peroxidase-like activity, which effectively catalyzes the oxidation of 2,2′-azino-bis(3-ethylbenzothiozoline-6-sulfonic acid) (ABTS) by H2O2 to produce the blue-green-colored free-radical cation (ABTS·+). Therefore, the detection of BLM can be achieved by observing the color transition with the naked eye or measuring the absorbance at a wavelength of 420 nm using a UV-Vis spectrophotometer. Attributing to the specific BLM-induced DNA strand scission and the effective locking of G-tetrads in the stem of the G4HP, the colorimetric sensing strategy exhibits high sensitivity and selectivity for detection of BLM in human serum samples, which might hold great promise for BLM assay in biomedical and clinical research.
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TALANTA
·
2022
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IF 6.556
Tongfu Huang,Mei Wang,Nian Hong,Hanfeng Cui,Qiqi Fan,Guobing Wei,Longshua Qin,Jing Zhang,Hao Fan
Herein, an autonomous driven DNA walker-based aptasensor is proposed for the detection of Ochratoxin A (OTA). A nanoscale metal-organic framework (MOF) is synthesized and used to load Mn 2+ , a cofactor for DNAzyme. The DNA walker and Mn 2+ @MOF are assembled on the Au surface, integrating the DNA walker and metal auxiliary ions. The proposed sensor avoids the addition of metal auxiliary ions of DNAzyme from the external environment, which achieves the fully autonomous driving of DNA walker and facilitates the on-site detection of OTA. In addition, the substrate strands are modified with a newly synthesized tetraferrocene signal marker, further achieving signal amplification. The sensor demonstrates a sensitivity of 0.289 pg/mL and is successfully applied to real food sample analysis.
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BIOMATERIALS
·
2021
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IF 12.479
Qi Xu,Hao Zhang,Hanghang Liu,Yaobao Han,Weibao Qiu,Zhen Li
Radio-resistance of glioblastoma (GBM) remains a leading cause of radiotherapy failure because of the protective autophagy induced by X-Ray irradiation and tumor cells’ strong capability of repairing damaged DNA . It is of great importance to overcome the radio-resistance for improving the efficacy of radiotherapy. Herein, we report the novel mechanism of core-shell copper selenide coated gold nanoparticles ( [email protected] 2- x Se NPs) inhibiting the protective autophagy and DNA repair of tumor cells to drastically boost the radiotherapy efficacy of glioblastoma. We reveal that the core-shell [email protected] 2- x Se NPs can inhibit the autophagy flux by effectively alkalizing lysosomes . They can increase the SQSTM1/p62 protein levels of tumor cells without influencing their mRNA. We also reveal that [email protected] 2- x Se NPs can increase the ubiquitination of DNA repair protein Rad51, and promote the degradation of Rad51 by proteasomes to prevent the DNA repair. The simultaneous inhibition of protective autophagy and DNA repair significantly suppress the growth of orthotopic GBM by using radiotherapy and our novel [email protected] 2- x Se NPs. Our work provides a new insight and paradigm to significantly improve the efficacy of radiotherapy by rationally designing theranostic nano-agents to simultaneously inhibit protective autophagy and DNA repair of tumor cells.
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ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Xiao-Qiong Li,Xiang-Nan Liu,Yi-Lei Jia,Xi-Liang Luo,Hong-Yuan Chen,Jing-Juan Xu
Lysosomal acidification is essential for its degradative function, and the flux of H+ correlated with that of K+ in lysosomes. However, there is little research on their correlation due to the lack of probes that can simultaneously image these two ions. To deeply understand the role of K+ in lysosomal acidification, here, we designed and fabricated a nanodevice using a K+-aptamer and two pH-triggered nanoswitches incorporated into a DNA triangular prism (DTP) as a dual signal response platform to simultaneously visualize K+ and pH in lysosomes by a fluorescence method. This strategy could conveniently integrate two signal recognition modules into one probe, so as to achieve the goal of sensitive detection of two kinds of signals in the same time and space, which is suitable for the detection of various signals with the correlation of concentration. By co-imaging both K+ and H+ in lysosomes, we found that the efflux of K+ was accompanied by a decrease of pH, which is of great value in understanding lysosomal acidification. Moreover, this strategy also has broad prospects as a versatile optical sensing platform for multiplexed analysis of other biomolecules in living cells.
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高影响因子
LANGMUIR
·
2021
·
IF 3.882
Xuelian Wang,Mei Liu,Xueqin Ding
Six hydrophobic magnetic guanidinium ionic liquids (HMILs) were designed and prepared for the extraction of DNA. The physical and thermal properties of the HMILs were characterized using vibrating sample magnetometry, density meter, rotational rheometer, Karl Fischer moisture, Fourier transform infrared spectrometry, and thermogravimetric analysis. Single-stranded DNA and duplex DNA extracted by HMILs can be rapidly collected by a magnet. Three assisted extraction methods, including vortex extraction, mechanical shaking extraction, and ultrasonic extraction, were introduced to extract DNA with HMILs and the extraction efficiencies were evaluated using NanoDrop. Influencing factors of the DNA extraction were comprehensively evaluated, involving the HMIL volume, extraction time, pH, and extraction temperature. The HMIL-based extraction method can well extract DNA from complex matrices and Escherichia coli cell lysates.
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ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Guo Liu,Shan Huang,Xiaochen Liu,Wanzhen Chen,Xin Ma,Shuang Cao,Liping Wang,Lanlan Chen,Huanghao Yang
Transmembrane signal transduction is of profound significance in many biological processes. The dimerization of cell-surface receptors is one prominent mechanism by which signals are transmitted across the membrane and trigger intracellular cascade amplification reactions. Recreating such processes in artificial systems has potential applications in sensing, drug delivery, bioengineering, and providing a new route for a deep understanding of fundamental biological processes. However, it remains a challenge to design artificial signal transduction systems working by the receptor dimerization mechanism in a predictable and smart manner. Here, benefitting from DNA with features of programmability, controllability, and flexible design, we use DNA as a building material to construct an artificial system mimicking dimerization of receptors for signal transduction and cascade amplification. DNA-based membrane-spanning receptor analogues are designed to recognize external signals, which drives two receptors into close spatial proximity to activate DNAzymes inside the cell-mimicking system. The activation of the DNAzyme initiates the catalyzed cleavage of encapsulated substrates and leads to the release of fluorescent second messengers for signal amplification. Such an artificial signal transduction system extends the range of biomimetic DNA-based signaling systems, providing a new avenue to study natural cell signaling processes and artificially regulate biological processes.
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