The excellent photophysical and electrochemical properties of porphyrins have inspired widespread interest in the realm of electrochemiluminescence (ECL). The aggregation-caused deficiency of ECL emission in aqueous solution, however, still severely impedes further applications. Herein, a molecule with a donor-acceptor (D-A) configuration, ATPP-Cou, consisting of monoaminoporphyrin as an electron donor and coumarin as an electron acceptor, was designed as an ECL luminophore to address the susceptibility of the porphyrin to aggregation-caused quenching (ACQ) in aqueous solution.
View Article and Find Full Text PDFRegulating the performance of peroxidase (POD)-like nanozymes is a prerequisite for achieving highly sensitive and accurate immunoassays. Inspired by natural enzyme catalysis, we design a highly active and selective nanozyme by loading atomically dispersed tungsten (W) sites on Pd metallene (W-O-Pdene) to construct an artificial three-dimensional (3D) catalytic center. The 3D asymmetric W-O-Pd atomic pairs can effectively stretch the O-O bonds in HO and further promote the desorption of HO to enhance POD-like activity.
View Article and Find Full Text PDFBecause of rapid industrialization and agriculturalization, solving the pressing problems of environment pollution, especially water and food quality, requires innovative solutions. In this paper, a novel and versatile metal-organic framework (ZIF-8)-hybrid monolithic column (ZIF-HMC) was prepared for in-tube solid-phase microextraction (IT-SPME) of organic nitrogen pesticides (ONPs). The prepared monolithic columns had superior adsorption sites, high porosity, excellent permeability, and ideal specific surface area based on Fourier Transform Infrared Spectroscopy (FT-IR), X-ray Diffraction (XRD), Thermal Field Emission Scanning Electron Microscopy (SEM), Energy Dispersive Spectrometry (EDS), X-ray Photoelectron Spectroscopy (XPS), and N adsorption-desorption.
View Article and Find Full Text PDFRational design of highly active and stable catalysts for dopamine oxidation is still a great challenge. Herein, inspired by the catalytic pocket of natural enzymes, an iodine (I)-doped single Fe-site catalyst (I/FeNC) is synthesized to mimic the catalytic center of heme enzymes in both geometrical and electronic structures, aiming to enhance dopamine (DA) oxidation. Experimental studies and theoretical calculations show that electronic communication between I and FeN effectively modulates the electronic structure of the active site, greatly optimizing the overlap of Fe 3d and O 2p orbitals, thereby enhancing OH adsorption.
View Article and Find Full Text PDFAn AND logic gate-based Hg ion colorimetric assay was constructed using the plasmonic and nanozyme dual signal channels of gold nanoparticles (AuNPs). This assay increased the judgment criteria for the identification of Hg ions and effectively improved the accuracy of Hg ion detection.
View Article and Find Full Text PDFNonylphenol (NP) is an important fine chemical raw material and intermediate that is widely utilized in industry and may be distributed in aquatic ecosystems. Following its entry into the food and water cycles, it can subsequently enter the human body and potentially harm the human reproductive system. For the purpose of monitoring NP in water, it is thus essential to build a straightforward, affordable, and robust electrochemical sensor.
View Article and Find Full Text PDFChem Commun (Camb)
August 2024
The development of dual linkage covalent organic frameworks (DL-COFs) is fundamentally important for creating diversified structures and functions. Herein, imine-hydrazone DL-COFs were synthesized for the first time. Three novel imine-hydrazone DL-COFs have been constructed with bifunctional molecule 4-amino-2-methoxybenzohydrazide as the key building block imine and hydrazone condensations simultaneously.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
November 2024
The electrochemical conversion of CO into valuable chemicals is a promising route for renowable energy storage and the mitigation of greenhouse gas emission, and production of multicarbon (C) products is highly desired. Here, we report a 1.4 %Pd-Cu@CuPz comprising of dispersive CuO and PdO dual nanoclusters embedded in the MOF CuPz (Pz=Pyrazole), which achieves a high C Faradaic efficiency (FE) of 81.
View Article and Find Full Text PDFBackground: Since the severe hazard to the ecosystem and widespread distribution through biological and man-made ways of polycyclic aromatic hydrocarbons (PAHs), it is very urgent to establish the ultrasensitive analytical method to quantitatively and directly monitor PAHs in real samples. However, because of the complicated environmental matrix and their trace concentration, the pre-concentration process is a necessary step to analyze of these compounds. In this study, solid phase microextraction (SPME) technique was proposed to separate and enrich fifteen trace PAHs from environmental samples.
View Article and Find Full Text PDFMetal-organic frameworks (MOFs) based composites with different structure-activity relationships have been widely used in the field of organic pollutant adsorption and extraction. Here, two MOF-on-MOF composites with different structures (yolk-shell and core-shell) from homologous sources were prepared by a simple in-situ growth synthesis method and structural regulation. In order to verify the effect of composite structure on the extraction capacity, the adsorption performance of the yolk-shell structure (YS-NH-UiO-66@CoZn-ZIF) and the core-shell structured (NH-UiO-66@CoZn-ZIF) material were compared by using them as coating material of direct immersion solid-phase microextraction (DI-SPME) to enrich six pesticides in five matrices.
View Article and Find Full Text PDFArtificial enzymes with high stability, adjustable catalytic activity, controllable preparation, and good reproducibility have been widely studied. Noble metal nanozymes, particularly gold nanoparticles (Au NPs), exhibit good catalytic activity, but their stability is poor. In this study, zeolitic imidazolate framework-8 (ZIF-8) was used as a carrier for Au NPs, thus improving the utilization efficiency and conservation stability of the nanozymes.
View Article and Find Full Text PDFRational design of peroxidase (POD)-like nanozymes with high activity and specificity still faces a great challenge. Besides, the investigations of nanozymes inhibitors commonly focus on inhibition efficiency, the interaction between nanozymes-involved catalytic reactions and inhibitors is rarely reported. In this work, we design a p-block metal Sn-doped Pt (p-d/PtSn) nanozymes with the selective enhancement of POD-like activity.
View Article and Find Full Text PDFAlthough oxygen reduction reaction (ORR) as an effective signal amplification strategy has been extensively investigated for the improvement of sensitivity of electrochemical sensors, their activity and stability are still a great challenge. Herein, single-atom Fe (FeSA) and Fe nanoparticles (FeNP) on nitrogen-doped carbon (FeSA/FeNP) catalysts demonstrate a highly active and stable ORR performance, thus achieving the sensitive and stable electrochemical sensing of organophosphorus pesticides (OPs). Experimental investigations indicate that FeNP in FeSA/FeNP can improve the ORR activity by adjusting the electronic structure of FeSA active sites.
View Article and Find Full Text PDFPesticides are common pollutants that cause detriment to the ecological environmental safety and health of human due to their toxicity, volatility and bioaccumulation. In this work, an ultra-thin polymetallic layered double hydroxide (FeCoNi-LDH) with hollow nanoflower structure composite was synthesized using ZIF-67 as a self-sacrificial template, which was used as solid-phase microextraction (SPME) coating for the targeted capture pesticides, which could be combined with high-performance liquid chromatography (HPLC) to sensitive inspection pesticides in real water samples. Orthogonal experimental design (OAD) was applied to ensure the best SPME condition.
View Article and Find Full Text PDFRadicals can feature theoretically 100% light utilization owing to their nonelectron spin-forbidden transition and represent the most advanced luminescent materials at present. 2,2,6,6-Tetramethyl-1-piperidinyloxy (TEMPO) acts as a typically stable radical with very broad applications. However, their luminescent properties have not been discovered to date.
View Article and Find Full Text PDFExploring novel electrochemiluminescence (ECL) molecules with high efficiency and good stability in aqueous solutions is crucial for achieving highly sensitive detection of analytes. However, developing chiral luminophores with efficient ECL performance is still a challenge. Herein, we first uncover that artemisinin (ART), a well-known chiral antimalarial drug, features a strong ECL emission at 726 nm with the assistance of a co-reactant potassium persulfate (KSO), and an ECL efficiency of 195.
View Article and Find Full Text PDFPharmaceuticals and personal care products (PPCPs) have a significant impact on the environment and human health, due to their sometimes toxic and carcinogenic characteristics. Therefore, an innovative chemosensor was constructed for ultrasensitive determination of two typical PCCPs (hydroquinone (HQ) and catechol (CC)) in several minutes. The homemade chemosensor (UiO-67@GO/MWCNTs) consisted of MOF(UiO-67), graphene oxide (GO), and multi-walled carbon nanotubes (MWCNTs) composites; it was a networked, structurally sparse, porosity-rich, homogeneous octahedral composite, and had ultra-high electrical conductivity, which provided lots of active adsorption sites, promote charge transfer, and enrich lots of molecules to be measured in a few minutes.
View Article and Find Full Text PDFNew strategies for accurate and reliable detection of adenosine triphosphate (ATP) with portable devices are significant for biochemical analysis, while most recently reported approaches cannot satisfy the detection accuracy and independent of large instruments simultaneously, which are unsuitable for fast, simple, and on-site ATP monitoring. Herein, a unique, convenient, and label-free point-of-care sensing strategy based on novel copper coordination polymer nanoflowers (CuCPNFs) was fabricated for multimode (UV-vis, photothermal, and RGB values) onsite ATP determination with high selectivity, sensitivity, and accuracy. The resulting CuCPNFs with a 3D hierarchical structure exhibit the ATP-triggered decomposition behavior because the competitive coordination between ATP and the copper ions of CuCPNFs can result in the formation of ATP-Cu, which reveals preeminent peroxidase mimics activity and can accelerate the oxidation of 3, 3', 5, 5'-tetramethylbenzidine (TMB) to form oxTMB.
View Article and Find Full Text PDFZnO quantum dots (QDs) supported on porous nitrogen-doped carbon (ZnO/P-NC) exhibited excellent electrochemical performance for the electroreduction of CO to CO with a faradaic efficiency of 95.3% and a current density of 21.6 mA cm at -2.
View Article and Find Full Text PDFNanozymes with peroxidase-like activity have been extensively studied for colorimetric biosensing. However, their catalytic activity and specificity still lag far behind those of natural enzymes, which significantly affects the accuracy and sensitivity of colorimetric biosensing. To address this issue, we design PdSn nanozymes with selectively enhanced peroxidase-like activity, which improves the sensitivity and accuracy of a colorimetric immunoassay.
View Article and Find Full Text PDFAs a fundamental product of CO conversion through two-electron transfer, CO is used to produce numerous chemicals and fuels with high efficiency, which has broad application prospects. In this work, it has successfully optimized catalytic activity by fabricating an electrocatalyst featuring crystalline-amorphous CoO-InO interfaces, thereby significantly expediting CO production. The 1.
View Article and Find Full Text PDFNanozymes with peroxidase (POD)-like activity have garnered significant attention due to their exceptional performance in colorimetric assays. However, nanozymes often possess oxidase (OD) and POD-like activity simultaneously, which affects the accuracy and sensitivity of the detection results. To address this issue, inspired by the catalytic pocket of natural POD, a single-atom nanozyme with FeN configuration is designed, exhibiting enhanced POD-like activity in comparison with a single-atom nanozyme with FeN configuration.
View Article and Find Full Text PDFBiVO is a promising photoanode for photoelectrochemical (PEC) water splitting but suffers from high charge carrier recombination and sluggish surface water oxidation kinetics that limit its efficiency. In this work, a model of sulfur-incorporated FeOOH cocatalyst-loaded BiVO was constructed. The composite photoanode (BiVO/S-FeOOH) demonstrates an enhanced photocurrent density of 3.
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