•A colorimetric aptasensor for the detection of multiple antibiotics is presented.•The method allows for multiplex antibiotics detection by the naked eye.•This colorimetric aptasensor displays great ...tolerance to high salt concentrations.•The method would promote the practical application via RGB analysis of smartphone.
We devise a novel colorimetric aptasensor for multiplex antibiotics based on an ss-DNA fragment coordinately controlling gold nanoparticles (AuNPs) aggregation. The multifunctional aptamer (Apt) was elaborately designed to be adsorbed on AuNPs surfaces acting as a binding element for antibiotics and a molecular switch. Chloramphenicol (CAP) and tetracycline (TET) were selected as the model antibiotics. When one kind of antibiotics was added, the specifically recognized fragment of Apt can bind to it and dissociated, and the non-specific one coordinately controls AuNPs aggregation under high-salt conditions. Hence, different color changes of AuNPs solution can be used as the signal readout. The aptasensor exhibited remarkable selectivity and sensitivity for separate detection of TET and CAP, and the detection limits are estimated to be 32.9 and 7.0 nM, respectively. The analysis with the absorption spectroscopy and the smartphone are applied to detect antibiotics in real samples with consistent results and desirable recoveries.
As emerging stimuli‐responsive materials, electrochromic metal‐organic frameworks (MOFs) are still not utilized in sensing applications due to difficulties in water stability, facile synthesis and ...functionalization, and efficient translation of specific recognition events. Here, we firstly find that a Zr‐based MOF furnished with postsynthetically created viologen‐like electron‐deficient moiety was electrochromic active. With a coordination‐driven surface engineering strategy where phosphate‐containing biomolecules are tethered to Zr nodes of the MOF, fine tuning the interface electron transfer was readily achieved, thus benefitting for constructing smart electrochromic sensors through the combination of the sensitivity of electrochemistry with the visuality of colorimetry. Particularly, MOF‐coated conductive films enabled label‐free detection of phosphoproteins, and aptamer‐functionalized ones responded specifically to the target. In two cases distinct color changes allow for visual quantification. This study represents the first example of MOF‐based electrochromic sensors developed by an efficient strategy, indicating the generality to electrochromic counterparts for various sensing applications.
By coordination‐driven surface engineering, an electrochromic Zr‐based metal‐organic framework incorporating a viologen‐like electron‐deficient moiety achieved modulated interface electron transfer, thus providing a favorable paradigm for visual analysis such as phosphoprotein detection and aptamer‐directed target recognition.
Tetracycline antibiotics (TCs) are one kind of broad spectrum bacteriostatic agents. However, excessive use of TCs will have a threat to the environment and human health. Therefore, it is necessary ...to develop a simple method for direct detection of TCs. Based on intrinsic peroxidase-like activity of gold nanoclusters (AuNCs), we used TC-specific aptamers (Apt) to improve the catalytic activity of AuNCs toward the peroxidase substrate 3,3′,5,5′-tetramethylbenzidine (TMB) oxidation by H2O2, and established a colorimetric sensing platform for TCs. The catalytic enhancement by Apt allows for sensitive colorimetric detection of TCs, and Apt as molecular recognition elements can specifically combine with TCs leading to high selectivity. This developed sensing platform can quantitatively detect TCs in the concentration range of 1–16 μM with a limit of detection (LOD) as low as 46 nM. Interestingly, the naked-eye detection capability of this method is estimated to be 0.5 μM. Finally, the detection of TCs in real samples like drugs and milk was validated.
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•A gold nanoclusters-based colorimetric aptasensor for tetracycline was presented.•Specificity and sensitivity of gold nanoclusters were greatly improved by aptamer.•The aptamer-enhanced peroxidase-like activity of gold nanoclusters was validated.•The sensor can accurately and reproducibly detect tetracycline in drugs and milk.
Concentration-dependent photoluminescence carbon dots (CDs) have been successfully synthesized through the one-step hydrothermal treatment of o-phthalic acid and ethylenediamine. The CDs possessed ...higher fluorescence quantum yield, up to 39.22%, exhibiting distinguished optical property, water solubility, and stability. The CDs that emit strong blue-green fluorescence can visually identify and determine tetracycline (TC), oxytetracycline (OTC), and chlortetracycline (CTC). TC quenched the fluorescence of CDs at 500 nm owing to the inner filter effect; OTC behaved similarly, but the emission wavelength of CDs was red-shifted to 515 nm. Inversely, once CTC was introduced to CDs solution, the fluorescence increased and the emission peak was blue-shifted to 450 nm. Bandgap transition and electrostatic interaction were proposed to be the mechanisms for the detection of OTC and CTC by CDs. Wide linear relationships were established for TC, OTC, and CTC with the limits of detection to be 50 nM, 36 nM, and 373 nM, respectively. Furthermore, the nanoscale probe constructed by this system has been applied to detect tetracyclines (TCs) in complex samples with satisfying recoveries (93.2–114%) and was designed as a portable test strip sensor for visually on-site TCs of honey sample screening. Accordingly, the preparation process of the nano fluorescent probe is simple and environmentally friendly, and the probe has a specific recognition ability for tetracyclines. The synthesized CDs in this work provide a new orientation for fast, effective, and visual real-time detection of tetracycline in actual samples.
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Lanthanide-based luminescent sensors have been widely used for the detection of the anthrax biomarker dipicolinic acid (DPA). However, mainly based on DPA sensitization to the lanthanide core, most ...of them failed to realize robust detection of DPA in bacterial spores. We proposed a new strategy for reliable detection of DPA by perturbing a tandem energy transfer in heterobinuclear lanthanide coordination polymer nanoparticles simply constructed by two kinds of lanthanide ions, Tb3+ and Eu3+, and guanosine 5′-monophosphate. This smart luminescent probe was demonstrated to exhibit highly sensitive and selective visual luminescence color change upon exposure to DPA, enabling accurate detection of DPA in complex biosystems such as bacterial spores. DPA release from bacterial spores on physiological germination was also successfully monitored in real time by confocal imaging. This probe is thus expected to be a powerful tool for efficient detection of bacterial spores in responding to anthrax threats.
Visual monitoring of the degradation of nerve agent simulants based on the switchable fluorescence of UiO-66-NH
2
was developed. In the hydrolysis, the decomposition products perturbed the ...linker-to-cluster charge transfer and stimulated the fluorescence recovery. Moreover, a "soft" solid-state platform utilizing agarose hydrogels was proposed to visualize the degradation of gaseous simulants without bulk water.
Visualizing the degradation of nerve agent simulants was achieved by stimulating the fluorescence recovery of UiO-66-NH
2
in solution and in the vapor phase.
Green production of NH3, especially the Li‐mediated electrochemical N2 reduction reaction (NRR) in non‐aqueous solutions, is attracting research interest. Controversies regarding the NRR mechanism ...greatly impede its optimization and wide applications. To understand the electrocatalytic process, we treated Au coated carbon fibrous paper (Au/CP) as the model catalyst. In situ XRD confirmed the transformation of lithium intermediates during NRR. Au greatly improved electron transfer kinetics to catalyze metallic Li formation, and accordingly highly accelerated spontaneous NRR. The Faradaic efficiency of NRR on Au/CP reached 34.0 %, and NH3 yield was as high as 50 μg h−1 cm−2. Our research shows that the key step of Li‐mediated non‐aqueous NRR is electrocatalytic Li reduction and offers a novel electrocatalyst design method for Li reduction.
The key step of Li‐mediated non‐aqueous NRR is electrocatalytic Li reduction. Gold greatly improved Li adsorption energy and thus highly accelerated the domino‐like nitrogen reduction reaction (NRR).
Molecular imprinting technology was used to coat polydopamine (PDA) onto MIL-53(Fe) surface by simple self-polymerization. The MIL-53(Fe)@MIP composite with enhanced peroxidase-like activity and ...specific target recognition function was synthesized and selected to construct a fluorescence sensor to detect metronidazole (MNZ). Since the substrate terephthalic acid was incorporated in the framework of MIL-53(Fe)@MIP, no additional luminescent substrate was required. This avoided the interference of the substrate on the enzymatic detection system and improved the accuracy of the assay. The characteristics of MIL-53(Fe)@MIP composite were investigated and confirmed by systematic analyses. The experimental results proved that the sensor provided satisfactory performances for quantitative determination of MNZ in wide linear range from 1 to 200 μM with low limit of detection as 53.4 nM. Potential interfering substances such as common cations and anions, amino acids, other antibiotics, sugars, and food additive were studied to show negligible effect on the assay, allowing the practical application to different fields including milk and human serum by the standard addition method. The recoveries were obtained between 93.2 and 102%, and the RSD was less than 3%.
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•MIL-53(Fe) capped with polydopamine was prepared by simple self-polymerization.•The composite had improved peroxidase activity and specificity to metronidazole.•No additional luminescent substrate was required, improving the assay accuracy.•The sensor showed high selectivity to metronidazole.•The sensor can accurately detect metronidazole in real samples.
α-Glucosidase, which directly involves in the metabolism of starch and glycogen and causes an increase in blood sugar level, is the major target enzyme for the precaution and therapy of type II ...diabetes. Based on the previous work, we adopted a post-synthetic modification method to encapsulate Tb3+ into Ce-MOF nanozyme which owned mixed valence states. Tb@Ce-MOF displayed induced luminescence characteristic and exceptional oxidase-like activity that could oxidize colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue ox-TMB. α-Glucosidase can hydrolyze the substrate l-ascorbic acid-2-O-α-d-glucopyranosyl (AAG) to generate ascorbic acid (AA), which could increase the Ce3+/Ce4+ redox valence mode in Tb@Ce-MOF, leading to the inhibition of the allochroic reaction of TMB and the decreased absorption of ox-TMB at 652 nm. The energy transfer (EnT) process from Ce3+ to Tb3+ will enhance due to the increased Ce3+/Ce4+ mode in Tb@Ce-MOF, which will result in an enhanced fluorescence signal of Tb@Ce-MOF at 550 nm. But the addition of inhibitor acarbose will inhibit the above process. We have constructed a dual-mode detection platform of α-glucosidase and its inhibitor via colorimetric and fluorometric method. The linear range of α-glucosidase were 0.01–0.5 U/mL (colorimetric mode) and 0.8–1.5 U/mL (fluorometric mode), respectively, with a detection limit as low as 0.0018 U/mL. Furthermore, our approach was also successfully employed to the analysis of α-glucosidase in serum samples.
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•Dual-mode nanoprobe was constructed based on Tb(Ⅲ)-modified Ce-MOF.•Tb@Ce-MOF exhibited intrinsic oxidase-like and induced luminescence properties.•The nanoprobe exhibited colorimetric and fluorometric response to α-glucosidase.•Dual-mode sensing platform enabled the accurate detection of α-glucosidase in human serum.
Here, using three metal cations (Mg
2+
, Al
3+
, and Zr
4+
) and an excited-state intramolecular proton transfer (ESIPT) active linker, 2,5-dihydroxyterephthalic acid (H
2
DHT), three luminescent ...metal-organic frameworks (LMOFs) were obtained. Importantly, their ESIPT-based luminescence originated from the linker was systematically tuned in emission profiles including intensity, emission color, and quantum efficiency in the solution as well as in the solid state, which is largely dependent on the composition and structural characteristics of these three LMOFs. Similar to the free linker, the Mg-based MOF possesses a relatively strong luminescence, the Al-based MOF has moderate luminescence due to the breathing effect, and the Zr-based MOF is very weakly luminescent, mainly caused by the LMCT process. Benefiting from unique emission behaviors of these three LMOFs, we further modulated their ESIPT-based luminescence through the interplay between guest species and components of LMOFs by combining with various photophysical processes, and successfully explored their potential applications as versatile photoluminescent platforms for target-triggered sensory materials, responsive fluorescent hydrogels, and white-light-emitting phosphors.
A systematic tuning of the emission profiles of an ESIPT luminophore incorporated in MOFs by varying metal nodes enables versatile photoluminescent applications.
