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1.
Herein, a cancer cell (MCF‐7 cell) membrane‐encapsulated dendritic mesoporous silica nanoparticle simultaneously functionalized with DNA‐photoacoustic (DNA‐PA) probes and glutathione (GSH)‐responsive DNA fuel strands for PA imaging of tumor‐related miRNA in living mice with signal amplification ability is developed. It is demonstrated that one target miRNA can trigger disassembly of multiple PA fluorophore probes from the quencher with the aid of GSH‐responsive DNA fuel strands via the entropy‐driven process, resulting remarkable amplified change of PA signal ratio. Using oncogenic miRNA‐21 as a model, a linear relationship between miRNA‐21 concentrations and PA ratio in a dynamic range from 10 × 10?12 m to 100 × 10?9 m and a limit of detection down to 11.69 × 10?12 m are established. The accurate PA signal observation related to miRNA‐21s in the tumor area in living mice is demonstrated, and the PA signal ratio increases significantly via the injection of miRNA‐21. It is anticipated that the catalytic ratiometric PA imaging system can be applied to an array of molecular detection in living system by rational detection probe design.  相似文献   

2.
Electrochemiluminescence (ECL) is a very sensitive method for trace analysis because of its background interference and high signal-to-noise ratio. In the past decade, the determination of Cu2+ in environment has attracted considerable attention since it plays an essential role in many physiological processes. Herein, a novel ECL sensor based on C,N quantum dots embedded g-C3N4 nanosheets (C,N-QDs@NSs) was constructed for the detection of Cu2+. The nanocomposite was rapidly obtained via the oxidation of normal g-C3N4 in H2O2 solution using sonochemical synthesizing method. Due to the abundant surface defects on C,N-QDs@NSs, the ECL intensity was magnified 2.5 times for using a C,N-QDs@NSs electrode in comparision to a g-C3N4 modified electrode. Besides, C,N-QDs@NSs could accelerate the rate of electron transfer in ECL reaction and thus resulted in the lower cathodic peak potential. Significantly, Cu2+ could effectively quench the ECL of C,N-QD@NSs, which endowed C,N-QD@NSs with a great advantage in the ECL detection of Cu2+. under optimum conditions, C,N-QDs@NSs modified electrode exhibited a linear detection range from 5 × 10?4 to 10 µM with a detection limit of 2 × 10?4 µM (S/N?=?3) for Cu2+, and was finally applied to detect Cu2+ in real samples with satisfactory results.  相似文献   

3.
It is a significant challenge to achieve controllable self‐assembly of superstructures for biological applications in living cells. Here, a two‐layer core–satellite assembly is driven by a Y‐DNA, which is designed with three nucleotide chains that hybridized through complementary sequences. The two‐layer core–satellite nanostructure (C30S5S10 NS) is constructed using 30 nm gold nanoparticles (Au NPs) as the core, 5 nm Au NPs as the first satellite layer, and 10 nm Au NPs as the second satellite layer, resulting in a very strong circular dichroism (CD) and surface‐enhanced Raman scattering. After optimization, the yield is up to 85%, and produces a g‐factor of 0.16 × 10?2. The hybridization of the target microRNA (miRNA) with the molecular probe causes a significant drop in the CD and Raman signals, and this phenomenon is used to detect the miRNA in living cells. The CD signal has a good linear range of 0.011–20.94 amol ngRNA?1 and a limit of detection (LOD) of 0.0051 amol ngRNA?1, while Raman signal with the range of 0.052–34.98 amol ngRNA?1 and an LOD of 2.81 × 10?2 amol ngRNA?1. This innovative dual‐signal method can be used to quantify biomolecules in living cells, opening the way for ultrasensitive, highly accurate, and reliable diagnoses of clinical diseases.  相似文献   

4.
Perovskite structured CsPbX3 (X = Cl, Br or I) quantum dots (QDs) have attracted great attention in the past few years for appealing application potentials in photovoltaic and optoelectronic devices. In this report, the CsPbX3 QDs are shown to perform as a new probe for metal ions with high sensitivity, high selectivity and instant response by the quenching or enhancing of the photoluminescence (PL). Through experimental and calculation efforts, the probing mechanisms are investigated. A wide probing window for Cu2+ and Yb3+ ions ranging from 2 × 10?9 to 2 × 10?6m is exhibited for CsPbBr3 QDs. In practice, the CsPbBr3 QDs are successfully applied for fast probing Cu2+ ions in edible oils and vehicle lubricating oils with the precision consistent to the values measured by inductively coupled plasma (ICP). Thus, it provides a promising powerful tool in detecting certain metal ions in biological and industrial organic solution systems.  相似文献   

5.
Exploring novel multifunctional rare earth materials is very important because these materials have fundamental interests, such as new structural facts and connecting modes, as well as potential technological applications, including optics, magnetic properties, sorption, and catalytic behaviors. Especially, employing these nanomaterials for sensing or catalytic reactions is still very challenging. Herein, a new superstable, anionic terbium‐metal–organic‐framework, [H2N(CH3)2][Tb(cppa)2(H2O)2], (China Three Gorges University ( CTGU‐1 ), H2cppa = 5‐(4‐carboxyphenyl)picolinic acid), is successfully prepared, which can be used as a turn‐on, highly‐sensitive fluorescent sensor to detect Eu3+ and Dy3+, with a detection limitation of 5 × 10?8 and 1 × 10?4m in dimethylformamide, respectively. This result represents the first example of lanthanide‐metal–organic‐frameworks (Ln‐MOF) that can be employed as a discriminative fluorescent probe to recognize Eu3+ and Dy3+. In addition, through ion exchanging at room temperature, Ag(I) can be readily reduced in situ and embedded in the anionic framework, which leads to the formation of nanometal‐particle@Ln‐MOF composite with uniform size and distribution. The as‐prepared Ag@ CTGU‐1 shows remarkable catalytic performance to reduce 4‐nitrophenol, with a reduction rate constant κ as large as 2.57 × 10?2 s?1; almost the highest value among all reported noble‐metal‐nanoparticle@MOF composites.  相似文献   

6.
Thin, adherent and stable polymeric films of 4-(2-pyridylazo)resorcinol (abbreviated as PPAR) were prepared by oxidative polymerization in 0.2 M NaOH solutions. PPAR films deposited on GC electrodes were found to inhibit the electron transfer reactions of the couple [Fe(CN)6]3?/4?. The redox behaviour of CuCl2 in 0.5 M KCl at bare and PPAR-covered GC electrodes was studied by cyclic voltammetry, RDE voltammetry and chronoamperometry. At PPAR-covered electrodes the peak potential of deposition of Cu occurs at ? 260 mV more cathodic potential than bare electrodes whereas the redox peaks of Cu2+/1+ and the oxidation of Cu → Cu1+ occur at the same potentials. Catalysis of thc redox processes of the couple Cu2+/1+ at PPAR-covered electrodes is attributed to incorporation of the redox species by chelation and electrostatic attraction. The diffusion coefficient of Cu2+ species (D = 0.29 × 10?5cm2 S?1) at PPAR-covered electrodes was found to be less than at bare electrodes (D = 0.95 × 10?5 cm2 S?1) whereas the effective bulk concentration (C = 28 mM) is higher than the used concentration: 10 mM.  相似文献   

7.
A highly efficient fluorescence gold nanoclusters probe for copper (II) (Cu2+) ions among various ions has been prepared through wool keratin as chelating and reducing agent. The main features of fluorescent gold nanoclusters supported on wool keratin (AuNCs@WK) probe are the high fluorescence in aqueous solution, the simplicity of synthesis and the hypotoxicity for living cells. The fluorescence probe exhibits high stability of pHs and shows more sensitivity under acidic condition. Upon exposure to various metal irons, only AuNCs@WK system with Cu2+ ions shows a fluorescence turnoff response changing from red to blue under UV light, which lead to the dramatically decreased fluorescent intensity of AuNCs@WK at 690 nm. Moreover, the high sensitivity of AuNCs@WK around 1 µM meets the need of detection standards. The slope of Stern–Volmer plot at low concentration of Cu2+ ions is greater than it at high concentrations, which indicates the aggregated AuNCs are from small amounts to large numbers with the increasing concentration of Cu2+ ions. The design mechanism of AuNCs@WK probe is the coordination of reactive groups to produce the complex (wool keratin-Cu-wool keratin) at 1:2 between Cu2+ ions and fluorescence probe. Furthermore, the cytotoxicity in cells indicates that AuNCs@WK system is safe for the selective imaging of copper ions in living cells.  相似文献   

8.
Two‐dimensional (2D) perovskites have proved to be promising semiconductors for photovoltaics, photonics, and optoelectronics. Here, a strategy is presented toward the realization of highly efficient, sub‐bandgap photodetection by employing excitonic effects in 2D Ruddlesden–Popper‐type halide perovskites (RPPs). On near resonance with 2D excitons, layered RPPs exhibit degenerate two‐photon absorption (D‐2PA) coefficients as giant as 0.2–0.64 cm MW?1. 2D RPP‐based sub‐bandgap photodetectors show excellent detection performance in the near‐infrared (NIR): a two‐photon‐generated current responsivity up to 1.2 × 104 cm2 W?2 s?1, two orders of magnitude greater than InAsSbP‐pin photodiodes; and a dark current as low as 2 pA at room temperature. More intriguingly, layered‐RPP detectors are highly sensitive to the light polarization of incoming photons, showing a considerable anisotropy in their D‐2PA coefficients (β[001][011] = 2.4, 70% larger than the ratios reported for zinc‐blende semiconductors). By controlling the thickness of the inorganic quantum well, it is found that layered RPPs of (C4H9NH3)2(CH3NH3)Pb2I7 can be utilized for three‐photon photodetection in the NIR region.  相似文献   

9.
Aqueous ion–solid interfacial interactions at an electric double layer (EDL) are studied in various research fields. However, details of the interactions at the EDL are still not fully understood due to complexity induced from the specific conditions of the solid and liquid parts. Several technical tools for ion–solid interfacial probing are experimentally and practically proposed, but they still show limitations in applicability due to the complicated measurements. Recently, an energy conversion device based on ion dynamics (called ionovoltaic device) was also introduced as another monitoring tool for the EDL, showing applicability as a novel probing method for interfacial interactions. Herein, a monitoring technique for specific ion adsorption (Cu2+ and Pb2+ in the range of 5 × 10?6–1000 × 10?6m ) in the solid–liquid interface based on the ionovoltaic device is newly demonstrated. The specific ion adsorption and the corresponding interfacial potentials profiles are also investigated to elucidate a working mechanism of the device. The results give the insight of molecular‐level ion adsorption through macroscopic water‐motion‐induced electricity generation. The simple and cost‐effective detection of the device provides an innovative route for monitoring specific adsorption and expandability as a monitoring tool for various solid–liquid interfacial phenomena that are unrevealed.  相似文献   

10.
Carbon dots (CDs), with excellent optical property and cytocompatibility, are an ideal class of nanomaterials applied in the field of biomedicine. However, the weak response of CDs in the near‐infrared (NIR) region impedes their practical applications. Here, UV–vis–NIR full‐range responsive fluorine and nitrogen doped CDs (N‐CDs‐F) are designed and synthesized that own a favorable donor‐π‐acceptor (D‐π‐A) configuration and exhibit excellent two‐photon (λex = 1060 nm), three‐photon (λex = 1600 nm), and four‐photon (λex = 2000 nm) excitation upconversion fluorescence. D‐π‐A‐conjugated CDs prepared by solvothermal synthesis under the assistance of ammonia fluoride are reported and are endowed with larger multiphoton absorption (MPA) cross sections (3PA: 9.55 × 10?80 cm6 s2 photon?2, 4PA: 6.32 × 10?80 cm8 s3 photon?3) than conventional organic compounds. Furthermore, the N‐CDs‐F show bright deep‐red to NIR fluorescence both in vitro and in vivo, and can even stain the nucleoli of tumor cells. A plausible mechanism is proposed on the basis of the strong inter‐dot and intra‐dot hydrogen bonds through N? H···F that can facilitate the expanding of conjugated sp2 domains, and thus not only result in lower highest occupied molecular orbital‐lowest unoccupied molecular orbital energy level but also larger MPA cross sections than those of undoped CDs.  相似文献   

11.
Metasurface serves as a promising plasmonic sensing platform for engineering the enhanced light–matter interactions. Here, a hyperbolic metasurface with the nanogroove structure in the subwavelength scale is designed. This metasurface is able to modify the wavefront and wavelength of surface plasmon wave with the variation of the nanogroove width or periodicity. At the specific optical frequency, surface plasmon polaritons are tightly confined and propagated with a diffraction‐free feature due to the epsilon‐near‐zero effect. Most importantly, the groove hyperbolic metasurface can enhance the plasmonic sensing with an ultrahigh phase sensitivity of 30 373 deg RIU?1 and Goos–Hänchen shift sensitivity of 10.134 mm RIU?1. The detection resolution for refractive index change of glycerol solution is achieved as 10?8 RIU based on the phase measurement. The detection limit of bovine serum albumin (BSA) molecule is measured as low as 0.1 × 10?18m (1 × 10?19 mol L?1), which corresponds to a submolecular detection level (0.13 BSA mm?2). As for low‐weight biotin molecule, the detection limit is estimated below 1 × 10?15m (1 × 10?15 mol L?1, 1300 biotin mm?2). This enhanced plasmonic sensing performance is two orders of magnitude higher than those with current state‐of‐art plasmonic metamaterials and metasurfaces.  相似文献   

12.
The interfacial reactions and mechanical properties of Sn-58Bi/Cu solder joints reflowed at different temperatures ranging from 180 to 220 °C for constant time of 10 min were investigated with various strain rates. Only a continuous Cu6Sn5 intermetallic compound (IMC) layer was formed at the interface between the Sn-58Bi solder and the Cu substrate during reflow. The equivalent thickness of the Cu6Sn5 layer increased with increasing reflow temperature, and the relationship between Cu6Sn5 layer equivalent thickness (X) and reflow temperature (T) is obtained by using method of linear regression and presented as $ X = 0.01 \times T + 0.187 $ . For the tensile property, the tensile strength of solder joint gradually decreased as the reflow temperature it increased, whereas it increased with increasing strain rate. Moreover, the fracture behavior of Sn-58Bi/Cu solder joint indicated the ductile fracture with low strain rate (5 × 10?4 and 1 × 10?3 s?1), while toward brittle fracture with high strain rate (2 × 10?3 and 1 × 10?2 s?1). The strain rate sensitivities of the solder joints fractured with various modes were also investigated, and it is found that the tensile strength of the solder is more sensitive to the strain rate than that of the IMC layer.  相似文献   

13.
We report X-ray diffraction and electron spin resonance (ESR) measurements of the effect of SrTiO3 ceramics doping using Cu2+ ions. ESR measurements reveal two kinds of Cu2+ centers in weakly (0.2–0.5 mol% Cu) doped SrTiO3. Both kinds of centers have been attributed to Cu2+ at octahedral Ti sites and possibly associated either with a nearest-neighboring oxygen vacancy (center #1) or some other positively charged defect (center #2). The ESR spectra of the above centers are described by the following spin Hamiltonian parameters: g  = 2.263(1), g  = 2.041(1), A  = 170(1) × 10?4 cm?1, A  = 27(1) × 10?4 cm?1 (center #1) and g  = 2.334(1), g  = 2.059(1), A  = 137(1) × 10?4 cm?1, A  ≈ 0(1) × 10?4 cm?1 (center #2). For copper concentration larger than 2 mol%, the antiferromagnetic SrCu3Ti4O12 (SCTO) phase has been detected by both X-ray diffraction and ESR. Its volume increases with increase of Cu concentration reaching about 17 % at Cu doping of 20 mol%. The composite SrTiO3–SCTO ceramics exhibits substantial magnetocapacitance effect, which could be enhanced by electrostriction of SrTiO3.  相似文献   

14.
Sensitive and selective detection of nitric oxide (NO) in the human body is crucial since it has the vital roles in the physiological and pathological processes. This study reports a new type of electrochemical NO biosensor based on zinc‐dithiooxamide framework derived porous ZnO nanoparticles and polyterthiophene‐rGO composite. By taking advantage of the synergetic effect between ZnO and poly(TTBA‐rGO) (TTBA = 3′‐(p‐benzoic acid)‐2,2′:5′,2″‐terthiophene, rGO = reduced graphene oxide) nanocomposite layer, the poly(TTBA‐rGO)/ZnO sensor probe displays excellent electrocatalytic activity and explores to detect NO released from normal and cancer cell lines. The ZnO is immobilized on a composite layer of poly(TTBA‐rGO). The highly porous ZnO offers a high electrolyte accessible surface area and high ion–electron transport rates that efficiently catalyze the NO reduction reaction. Amperometry with the modified electrode displays highly sensitive response and wide dynamic range of 0.019–76 × 10?6m with the detection limit of 7.7 ± 0.43 × 10?9m . The sensor probe is demonstrated to detect NO released from living cells by drug stimulation. The proposed sensor provides a powerful platform for the low detection limit that is feasible for real‐time analysis of NO in a biological system.  相似文献   

15.
A newly developed electrochemical biosensor composed of a topological insulator (TI) and metallic DNA (mDNA) is fabricated. The bismuth selenide nanoparticle (Bi2Se3 NP) is synthesized and sandwiched between the gold electrode and another Au‐deposited thin layer (Bi2Se3@Au). Then, eight‐silver‐ion mediated double‐stranded DNA (mDNA) is immobilized onto the substrate (Bi2Se3@Au‐mDNA) for the further detection of hydrogen peroxide. The Bi2Se3 NP acts as the electrochemical‐signal booster, while unprecedentedly its encapsulation by the Au thin layer keeps the TI surface states protected, improves its electrochemical‐signal stability and provides an excellent platform for the subsequent covalent immobilization of the mDNA through Au–thiol interaction. Electrochemical results show that the fabricated biosensor represents much higher Ag+ redox current (≈10 times) than those electrodes prepared without Bi2Se3@Au. The characterization of the Bi2Se3@Au‐mDNA film is confirmed by atomic force microscopy, scanning tunneling microscopy, and cyclic voltammetry. The proposed biosensor shows a dynamic range of 00.10 × 10?6m to 27.30 × 10?6m , very low detection limit (10 × 10?9m ), unique current response (1.6 s), sound H2O2 recovery in serum, and substantial capability to classify two breast cancer subtypes (MCF‐7 and MDA‐MB‐231) based on their difference in the H2O2 generation, offering potential applications in the biomedicine and pharmacology fields.  相似文献   

16.
Herein, a versatile and sensitive colorimetric sensor for Hg2+ based on aptamer–target specific binding and target‐mediated growth of AuNPs is reported. The 15 T bases are first designed to detect Hg2+ through T–Hg2+–T coordination. Aptamer–target binding results in the desorption of the aptamer from AuNP surface, the remaining aptamers adsorbed on AuNP surface trigger the growth of AuNPs with morphologically varied nanostructures, and then different colored solutions are formed. On this occasion, the limit of detection (LOD) of 9.6 × 10?9m is obtained. The other two aptamer strands (25‐ and 59‐mer) are designed by increasing A bases on either side and both sides of 15 T, respectively. The interaction of the binding domain and Hg2+ makes desorption of 15 T from AuNP surface, whereas excess bases not committed to the binding domain still adsorbed on AuNP surface. These excess bases control the growth of AuNPs, and enhance the sensitivity. The LODs are 4.05 and 3 × 10?9m for 25‐ and 59‐mer aptamers, respectively. In addition, the 59‐mer aptamer system is applied to identify Hg2+ in real river samples, the LOD of 6.2 × 10?9m is obtained.  相似文献   

17.
In situ monitoring of hydrogen peroxide (H2O2) during its production process is needed. Here, an electrochemical H2O2 sensor with a wide linear current response range (concentration: 5 × 10?8 to 5 × 10?2 m ), a low detection limit (32.4 × 10?9 m ), and a high sensitivity (568.47 µA mm ?1 cm?2) is developed. The electrocatalyst of the sensor consists of cobalt nanoparticles and atomic Co‐Nx moieties anchored on nitrogen doped carbon nanotube arrays (Co‐N/CNT), which is obtained through the pyrolysis of the sandwich‐like urea@ZIF‐67 complex. More cobalt nanoparticles and atomic Co‐Nx as active sites are exposed during pyrolysis, contributing to higher electrocatalytic activity. Moreover, a portable screen‐printed electrode sensor is constructed and demonstrated for rapidly detecting (cost ≈40 s) H2O2 produced in microbial fuel cells with only 50 µL solution. Both the synthesis strategy and sensor design can be applied to other energy and environmental fields.  相似文献   

18.
The present study is focused on the copper-doped ZnO system. Bulk copper-doped ZnO pellets were synthesized by a solid-state reaction technique and used as target material in pulsed laser deposition. Thin films were grown for different Cu doped pellets on sapphire substrates in vacuum (5×10?5 mbar). Thin films having (002) plane of ZnO showed different oxidation states of dopants. MH curves exhibited weak ferromagnetic signal for 1–3 % Cu doping but for 5 % Cu doped thin film sample showed the diamagnetic behavior. For deeper information, thin films were grown for 5 % Cu doped ZnO bulk pellet in different oxygen ambient pressures and analyzed. PL measurement at low temperature showed the emission peak in thin films samples due to acceptor-related transitions. XPS results show that copper exists in Cu2+ and Cu+1 valence states in thin films and with increasing O2 ambient pressure the valence-band maximum in films shifts towards higher binding energy. Furthermore, in lower oxygen ambient pressure (1×10?2 mbar) thin films showed magnetic behavior but this vanished for the film grown at higher ambient pressures of oxygen (6×10?2 mbar), which hints towards the decrease in donor defects.  相似文献   

19.
The integration of graphene with colloidal quantum dots (QDs) that have tunable light absorption affords new opportunities for optoelectronic applications as such a hybrid system solves the problem of both quantity and mobility of photocarriers. In this work, a hybrid system comprising of monolayer graphene and self‐doped colloidal copper phosphide (Cu3?x P) QDs is developed for efficient broadband photodetection. Unlike conventional PbS QDs that are toxic, Cu3?x P QDs are environmental friendly and have plasmonic resonant absorption in near‐infrared (NIR) wavelength. The half‐covered graphene with Cu3?x P nanocrystals (NCs) behaves as a self‐driven p–n junction and shows durable photoresponse in NIR range. A comparison experiment reveals that the surface ligand attached to Cu3?x P NCs plays a key role in determining the charge transfer efficiency from Cu3?x P to graphene. The most efficient three‐terminal photodetectors based on graphene‐Cu3?x P exhibit broadband photoresponse from 400 to 1550 nm with an ultrahigh responsivity (1.59 × 105 A W?1) and high photoconductive gain (6.66 × 105) at visible wavelength (405 nm), and a good responsivity of 9.34 A W?1 at 1550 nm. The demonstration of flexible graphene‐Cu3?x P photodetectors operated at NIR wavelengths may find potential applications in optical sensing, biological imaging, and wearable devices.  相似文献   

20.
In this study, a CuxOS@ZIF-8 nanostructure is fabricated to quantify the levels of hydrogen sulfide (H2S) in living cells and in vivo. Zeolitic lmidazolate framework-8 (ZIF-8) is chosen as an encapsulation shell to improve the selectivity of this probe. Using this unique nanostructure, ultrasensitive quantification and bioimaging of H2S in living cells are successfully achieved. The lower limit of detection is 0.8 and 5.3 nmol per 106 cells for circular dichroism and fluorescence modes, respectively. It is found that the chiral CuxOS NPs transformed into achiral CuxS NPs contribute to the ultrasensitive detection. Notably, this probe can also be carried out to detect and track H2S levels in tumor-bearing animals. The discoveries put forward for the creation of a detection platform for quantitative tracking and analysis in clinic.  相似文献   

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