Receptors are crucial to the analytical performance of sensor arrays. Different from the previous receptors in sensor arrays, herein, peroxidase-mimicking DNAzymes were innovatively used as receptors ...to develop a label-free chemiluminescence sensor array for discriminating various heavy metal ions in complex samples. The peroxidase-mimicking DNAzymes are composed of functional oligonucleotides and hemin, including G-triplex-hemin DNAzyme (G3-DNAzyme), G-quadruplex-hemin DNAzyme (G4-DNAzyme), and the dimer of G-quadruplex-hemin DNAzyme (dG4-DNAzyme). Circular dichroism (CD) spectroscopy demonstrated that different metal ions diversely affect the conformation of G-quadruplex and G-triplex, resulting in a change in the activity of peroxidase-mimicking DNAzyme. Thus, the unique fingerprints formed to easily discriminate seven kinds of heavy metal ions by principal component analysis (PCA) within 20 min. The discrimination of unknown metal ions in tap water further confirmed its ability for discriminating multiple heavy metal ions. Moreover, it will not bring water pollution due to the good biocompatibility of DNA. Therefore, it not only merely offers a label-free, rapid, environment-friendly, and cheap (1.49 $) sensor assay for discriminating metal ions but also comes up with an innovative way for developing sensor arrays.
The upregulation of microRNA (miRNA) is highly related with some kinds of tumor, such as breast, prostate, lung, and pancreatic cancers. Therefore, for an important tumor biomarker, the point-of-care ...testing (POCT) of miRNA is of significant importance and is in great demand for disease diagnosis and clinical prognoses. Herein, a POCT assay for miRNA detection was developed via a portable pressure meter. Two hairpin DNA probes, H1 and H2, were ingeniously designed and functionalized with magnetic beads (MBs) and platinum nanoparticles (PtNPs), respectively, to form MBs-H1 and PtNPs-H2 complexes. In the presence of target microRNA 21 (miR-21), the cyclic strand displacement reaction (SDR) between MBs-H1 and PtNPs-H2 was triggered to continuously form the MBs-H1/PtNPs-H2 duplex. Owing to the amplification of cyclic SDR, numerous PtNPs were enriched onto the surface of MBs to catalytically decompose H2O2 for the generation of much O2. The gas pressure value has a linear relationship with the logarithmic value of miR-21 concentration in the range of 10 fM to 10 pM. The limit of detection is 7.6 fM, which is more sensitive than that in a number of previous reports. Hairpin DNA probes and magnetic separation highly ensured the specificity and reliability. Single-base mutation was easily discriminated, and the detection of miR-21 in the serum sample achieved satisfactory result. Therefore, it offers a reliable POCT strategy for the detection of miRNA, which is of great theoretical and practical importance for POCT clinical diagnostics.
Many current chemodynamic therapy (CDT) strategies suffer from either low therapeutic efficiency or the deficiency of poor targeting. The low therapeutic efficiency is mainly ascribed to the ...intracellular antioxidant system and the inefficient Fenton reaction in the weakly acidic tumor microenvironment (TME). Herein, by exploitation of the diverse function and programmability of functional nucleic acid, aptamer-tethered nanotrains of DNA copper nanoclusters (aptNTDNA-CuNCs) were assembled to simultaneously achieve targeted recognition, loading, and delivery of CDT reagents into tumor cells without an external carrier. The intracellular hydrogen peroxide (H2O2) oxidized nanotrains of DNA-CuNCs to produce a lot of Cu2+ and Cu+ ions, which can generate reactive oxygen species (ROS) in the weakly acidic TME based on the pH-independent Fenton-like reaction of Cu+/H2O2. Meanwhile, the redox reaction between intracellular glutathione (GSH) and Cu2+ depleted GSH and generated Cu+ ions, which weakened the antioxidant ability of cancer cells and further enhanced the Fenton-like reaction of Cu+/H2O2, respectively. Thus, the cascade Fenton-like reaction and GSH depletion doubly improved the efficacy of CDT. The in vivo and in vitro study solidly confirmed that aptNTDNA-CuNCs have excellent antitumor efficacy and no cytotoxicity to healthy cells. Therefore, aptNTDNA-CuNCs can act as CDT reagents to achieve highly efficient, biocompatible, and targeted CDT.
Molecular logic gate provides an intelligent option for simultaneous detection of biomarkers. Herein, a dual-mode DNA logic gate was proposed to portably and intelligently detect multiple microRNAs ...(miRNAs) by gas pressure biosensing and lateral flow assay (LFA). A platinum-coated gold nanoparticle (Au@PtNP) with catalase-like activity was used as a signal reporter to achieve a dual-signal readout. MiRNAs as the input initiated the cyclic strand displacement reaction (SDR) to enrich a large amount of Au@PtNPs. Thus, miRNA can be visually detected by a lateral flow strip (LFS) using the grayish-brown color of Au@PtNPs as output 1. Furthermore, Au@PtNP-catalyzed decomposition of H2O2 resulted in gas pressure as output 2, which was measured by a digital and handheld gas pressure meter. As a consequence, microRNA 21 (miR-21) was sensitively and reliably detected with the limit of detection (LOD) of 7.2 pM. The selectivity and real sample analysis were both satisfactory. Significantly, two-input and three-input AND logic gates were successfully developed to realize multiple detection of two miRNAs and three miRNAs, which provide a promising way for intelligent multi-input analysis. Predictably, with the advantages of portability, simplicity, and affordability, the dual-mode logic gate based on gas pressure biosensing and LFA offers a new perspective on the field of intelligent and portable biosensing and bioanalysis.
Simultaneous detection of multi-biomarkers not only enhances the accuracy of disease diagnosis but also improves detection efficiency and reduces cost. It is vital to achieve portable, simple, ...low-cost, and simultaneous detection of biomarkers for point-of-care (POC) diagnostics in a low-resource setting. Herein, a multichannel paper chip-based gas pressure bioassay was developed for the simultaneous detection of multiple biomarkers by combining multichannel paper chips with a portable gas pressure meter. Four DNA tetrahedral probes (DTPs) were used as capture probes and were immobilized in different detection zones of the paper chips to improve hybridization efficiency and reduce nonspecific adsorption. The formation of a sandwich structure between target microRNAs (miRNAs), the capture probe, and platinum nanoparticles (PtNPs)-modified complementary DNA (PtNPs-cDNA) transformed biomolecular recognition into quantitative detection of gas pressure. Four lung cancer-related miRNAs were detected simultaneously by a portable gas pressure meter. There is a good linear relationship between gas pressure and the logarithm of miRNA concentration in the range of 10 pM to 100 nM. Compared with single-stranded DNA capture probe, the signal-to-noise (S/N) of DNA tetrahedral probes improved more than 3 times. Using ring-oven washing, the unbound reagents in all channels of the paper chip were simultaneously and continuously washed away, leading to a more cheap, simple, and fast separation than magnetic separation. Therefore, it offers a promising multichannel paper chip-based gas pressure bioassay for portable and simultaneous detection of multiple biomarkers.
To improve the ignition and combustion characteristics and combustion efficiency of micron-sized aluminum particle in high temperature water vapor atmosphere, a self-designed tube furnace setup was ...used to study the effects of potassium fluoride (KF) on the ignition and combustion characteristics of micron-sized aluminum particle in high temperature water vapor. The ignition and combustion processes, components and morphologies of combustion products, and combustion efficiency were recorded and analyzed by a high-speed photographic system, X-ray diffraction, scanning electron microscopy with energy-dispersive spectrometer, and chemical analysis method, respectively. Results show that the addition of KF to 5 μm aluminum powder significantly decreases its ignition delay time because the hydrolysis of KF generates KOH in water vapor, and KOH corrodes the oxide shell on the aluminum surface to promote the reaction of aluminum with water, which can be proved by the morphologies of the products. The hydrolysis product of KF can destroy the oxidation shell on the aluminum powder surface, but it does not cause the aluminum particles to undergo shell-breaking combustion. As the KF content increases, the oxide shell is dramatically destroyed, so the ignition delay time of aluminum powder in high temperature water vapor decreases. Moreover, the combustion efficiency of aluminum powder with addition of KF increases considerably with increasing of the KF content.
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•The ratiometric FRET successfully and reliably detected intracellular hTR.•Ratiometric FRET and hairpin structure of DNA probes ensured the specific detection of hTR.•Fluorescent ...imaging reliably identified the difference in the expression level of hTR between cancer cells and normal cells.
Human telomerase RNA (hTR) is one essential component of telomerase and is overexpressed in tumor cells. Therefore, the reliable and sensitive detection of hTR is essential for the early cancer diagnosis. Herein, to avoid the false positive signals caused by co-existing components in the cell, a ratiometric fluorescence resonance energy transfer (FRET) strategy was developed to achieve reliable detection of intracellular hTR. Manganese dioxide nanosheets (MnO2NS) with good biocompatibility carry two fluorophore-labelled hairpin DNA probes into the cancer cell and then release the probes via decomposition of MnO2NS by intracellular L-glutathione reduced (GSH). Then, hTR triggered the cyclic strand displacement reaction (SDR) between two hairpin DNA probes to continuously form DNA duplexes, which made two fluorophores close to each other and led to an effective FRET. Fluorescence imaging demonstrated a higher expression level of hTR in HeLa cells than that in normal HL-7702 cells. The high specificity of hairpin DNA probes and SDR make it easy to discriminate the single-base mutation. Therefore, it provides a highly sensitive, simple and reliable method for the extracellular and intracellular detection of hTR.
Cross-reactive sensor arrays are useful for discriminating multiple analytes in a complex sample. Herein, a portable and label-free gas pressure sensor array was proposed for multiplex analysis via a ...handheld gas pressure meter. It is based on the interaction diversity of analytes with catalase-like nanomaterials, including Pt nanoparticles (PtNP), Co3O4 nanosheets (Co3O4NS), and Pt–Co alloy nanosheets (PtCoNS), respectively. Thus, the diverse influence of analytes on the catalase-like activity could be output as the difference in the gas pressure. By using principal component analysis, eight proteins were well distinguished by the gas pressure sensor array at the 10 nM level within 12 min. Moreover, different concentrations of proteins and mixtures of proteins could likewise be discriminated. More importantly, the effective discrimination of proteins in human serum and discrimination of five kinds of cells further confirmed the potential of the gas pressure sensor array. Therefore, it provides a portable, cheap, sensitive, and label-free gas pressure sensor array, which is totally different from the reported sensor arrays and holds great potential for portable and cheap discrimination of multiple analytes.
As a natural green catalyst, laccase has extensive application in the fields of environmental monitoring and pollutant degradation. However, susceptibility to environmental influences and poor ...reusability seriously hinder its application. To address these concerns, for the first time, manganese ion replaced copper ion as the active center to coordinate with guanosine monophosphate (GMP) for synthesizing mimic laccase with high catalytic activity. Compared with natural laccase, the laccase-like nanozyme (Mn–GMPNS) demonstrated superior thermal stability, acid–base resistance, salt tolerance, reusability, and substrate universality. Benefiting from the high catalytic activity of Mn–GMPNS, epinephrine, a significant neurotransmitter and hormone associated with numerous diseases, was visually detected within 10 min and a portable assay by smartphone. More encouragingly, Mn–GMPNS can efficiently degrade dye pollutants, achieving a decolorization rate over 70% within 30 min. Thus, the coordination between manganese ion and nucleotide demonstrated the potential in rational design of nanozymes with high catalytic activity, low cost, good stability, and good biocompatibility.
DNA logic gates have shown outstanding magic in intelligent biology applications, but it remains challenging to construct a portable, affordable and convenient DNA logic gate. Herein, logic gates of ...gas pressure were innovatively developed for multiplex analysis of metal ions. Hg2+ and Ag+ were input to interact specifically with the respective mismatched base pairs, which activated DNA extension reaction by polymerase and led to the enrichment of platinum nanoparticles for catalyzing the decomposition of peroxide hydrogen. Thus, the gas pressure obtained from a sealed well was used as output for detecting or identifying metal ions. Hg2+ and Ag+ were sensitively and selectively detected, and the assay of the real samples was also satisfactory. Based on this, DNA logic gates, including YES, NOT, AND, OR, NAND, NOR, INHIBIT, and XOR were successfully established using a portable and hand-held gas pressure meter as detector. So, the interactions between DNA and metal ions were intelligently transferred into the output of gas pressure, which made metal ions to be detected portably and identified intelligently. Given the remarkable merits of simplicity, logic operation, and portable output, the metal ion-driven DNA logic gate of gas pressure provides a promising way for intelligent and portable biosensing.
