Nowadays, aggregation-caused quenching (ACQ) of organic molecules in aqueous media seriously restricts their analytical and biomedical applications. In this work, hydrogen bond (H-bond) was utilized to resist the ACQ effect of 2,5,8-triamino-1,3,4,6,7,9,9b-heptaazaphenalene (Melem) as an advanced electrochemiluminescence (ECL) luminophore, whose ECL process was carefully studied in an aqueous KSO system coupled with electron paramagnetic resonance (EPR) measurements. Notably, the H-bond-induced Melem assemblies (Melem-H) showed 16.
View Article and Find Full Text PDFNowadays, continuous efforts have been devoted to designing stable and high-efficiency electrochemiluminescence (ECL) emitters as alternatives for tris(2,2'-bipyridine)-ruthenium(II) (Ru(bpy)) in medical research. Herein, a novel ECL emitter was obtained by coordinating crystalline covalent triazinyl frameworks (cCTFs) with Ru (termed Ru-cCTFs), which exhibited strong ECL emission by the ligand to metal charge transfer (LMCT) route. After its integration with 4-mercaptopyridine (SH-Py), the resultant SH-Py-Ru-cCTFs achieved 2.
View Article and Find Full Text PDFNowadays, signal enhancement is imperative to increase sensitivity of advanced ECL devices for expediting their promising applications in clinic. In this work, photodynamic-assisted electrochemiluminescence (PDECL) device was constructed for precision diagnosis of Parkinson, where an advanced emitter was prepared by electrostatically linking 2,6-dimethyl-8-(3-carboxyphenyl)4,4'-difluoroboradiazene (BET) with 1-butyl-3-methylimidazole tetrafluoroborate ([BMIm][BF]). Specifically, protoporphyrin IX (PPIX) can trigger the photodynamic reaction under light irradiation with a wavelength of 450 nm to generate lots of singlet oxygen (O), showing a 2.
View Article and Find Full Text PDFNowadays, novel and efficient signal amplification strategy in electrochemiluminescence (ECL) platform is urgently needed to enhance the sensitivity of biosensor. In this work, the dual ECL signal enhancement strategy was constructed by the interactions of Pd nanoparticles attached covalent organic frameworks (Pd NPs@COFs) with tris (bipyridine) ruthenium (RuP) and Exonuclease III (Exo.III) cycle reaction.
View Article and Find Full Text PDFNowadays, organic emitters suffer from insufficient electrochemiluminescence (ECL) efficiency in aqueous solutions, and their practical applications are severely restricted in the bio-sensing field. In this work, palladium nanospheres-embedded metal-organic frameworks (Pd@MOFs) were exploited to enhance the ECL efficiency of 2,6-dimethyl-8-(3-carboxyphenyl)4,4'-difluoroboradiazene (BET) prepared by a one-pot method in aqueous environment. First, the Pd@MOFs were generated reduction of Pd nanospheres anchored onto the MOFs, and fabricated by orderly coordination of palladium chloride (PdCl) with 1,2,4,5-benzenetetramine (BTA) tetrahydrochloride.
View Article and Find Full Text PDFElectrochemiluminescence (ECL) has attracted significant interest in the analysis of cancer cells, where the ruthenium(II)-based emitter demonstrates urgency and feasibility to improve the ECL efficiency. In this work, the self-enhanced ECL luminophore was prepared by covalent anchoring of Pd nanoclusters on aminated metal organic frameworks (Pd NCs@MOFs), followed by linkage with bis(2,2'-bipyridine)-5-amino-1,10-phenanthroline ruthenium(II) (RuP). The resultant luminophore showed 214-fold self-magnification in the ECL efficiency over RuP alone, combined by promoting the interfacial photoelectron transfer.
View Article and Find Full Text PDFAccurate intracellular cholesterol traffic plays crucial roles. Niemann Pick type C (NPC) proteins NPC1 and NPC2, are two lysosomal cholesterol transporters that mediate the cholesterol exit from lysosomes. However, other proteins involved in this process remain poorly defined.
View Article and Find Full Text PDFNowadays, synthesis of novel organic photosensitizer is imperative but challenging for photoelectrochemical (PEC) assay in analytical and biomedical fields. In this work, the PEC responses enhanced about 4.3 folds after in situ electrostatic assembly of 1-butyl-3-methylimidazole tetrafluoroborate ([BIm][BF]) on meso-tetra (4-carboxyphenyl) porphine (TP), which was first covalently linked with NH modified indium tin oxide electrode ([BIm]-TP-NH-ITO).
View Article and Find Full Text PDFNowadays, electrochemiluminescence (ECL) efficiency of an organic emitter is closely related with its potential applications in food safety and environmental monitoring fields. In this work, 2,4,6-tris(4-carboxyphenyl)-1,3,5-triazine (TATB) was self-assembled to form hydrogen bond organic frameworks (HOFs), which worked as ideal reactors to generate highly active oxygen-containing radicals, followed by linking with isoluminol (ILu) via amide bond (termed ILu-HOFs). After covalent assembly with aminated indium-tin oxide electrode (labeled NH-ITO), the ECL efficiency of the ILu-HOFs NH-ITO showed about a 23.
View Article and Find Full Text PDFCytochrome (cyt ) plays a critical role in mitochondrial respiratory chain, whose absence is detrimental to electron transport and reduce adenosine triphosphate. For ultrasensitive detection of cyt , sheet-like covalent organic frameworks (COFs) were prepared by orderly accumulation of 1,3,5-benzenetricarboxaldehyde (BTA) and -phenylenediamine (PDA), and further grafted with -(4-aminobutyl)--ethylisoluminol (ABEI) - an electrochemiluminescence (ECL) emitter. Specifically, the morphology and structure of the COFs-ABEI were mainly characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD) analysis, and X-ray photoelectron spectroscopy (XPS).
View Article and Find Full Text PDFHeterometallic nanomaterials (HMNMs) display superior physicochemical properties and stability to monometallic counterparts, accompanied by wider applications in the fields of catalysis, sensing, imaging, and therapy due to synergistic effects between multi-metals in HMNMs. So far, most reviews have mainly concentrated on introduction of their preparation approaches, morphology control and applications in catalysis, assay of heavy metal ions, and antimicrobial activity. Therefore, it is very important to summarize the latest investigations of activity modulation of HMNMs and their recent applications in sensing, imaging and therapy.
View Article and Find Full Text PDFNowadays, aggregation quenching of most organic photosensitizers in aqueous media seriously restricts analytical and biomedical applications of photoelectrochemical (PEC) sensors. In this work, an aggregation-enhanced PEC photosensitizer was prepared by electrostatically bonding protoporphyrin IX (PPIX) with an ionic liquid of 1-butyl-3-methylimidazole tetrafluoroborate ([BMIm][BF]), termed as PPIX-[BMIm] for clarity. The resultant PPIX-[BMIm] showed weak photocurrent in pure dimethyl sulfoxide (DMSO, good solvent), while the PEC signals displayed a 44.
View Article and Find Full Text PDFNowadays, continuous efforts have been devoted to searching highly efficient electrochemiluminescence (ECL) emitters for applications in clinical diagnosis and food safety. In this work, triazinyl-based hydrogen bond organic frameworks (Tr-HOFs) were synthesized by N···H hydrogen bond self-assembly aggregation, where 6,6'-(1,4-phenylene)bis(1,3,5-triazine-2,4-diamine) (phenyDAT) was prepared the cyclization reaction and behaved as a novel ligand. Impressively, the resulting Tr-HOFs showed strong ECL responses with highly enhanced ECL efficiency (21.
View Article and Find Full Text PDFNowadays, brain natriuretic peptide (BNP-32) is fundamental to early cardiovascular clinical diagnosis, whose accurate assay is of significance by photoelectrochemistry (PEC) for the low background and high precision. Herein, a novel enhanced PEC platform was built by successive deposition of N-doped ZnO nanopolyhedra (N-ZnO NP) and protoporphyrin IX (PPIX). Specifically, the N-ZnO NP with a narrow bandgap of 2.
View Article and Find Full Text PDFIn this work, metal-organic frameworks (MOFs) are utilized as effective ECL coreactant accelerator to enhance the ECL responses of -(aminobutyl)--(ethylisoluminol) (ABEI). Zn-based MOFs (MOF-Zn-1) were prepared by chelating Zn ions with melamine and thiophenedicarboxylic acid (TPDA), which observably accelerated the electrocatalytic oxidation of tripropylamine (TPA). Then, ABEI-MOF-Zn-1 as a high-performance ECL emitter was synthesized an amide reaction between ABEI and mercaptopropionic acid (MPA) modified MOF-Zn-1.
View Article and Find Full Text PDFExploring advanced nanocatalysts are of importance for hydrogen evolution reaction (HER) in alkaline electrolyte (e.g. 1.
View Article and Find Full Text PDFDevelopment of ultra-sensitive and high specific aptasensors is important for early diagnosis of prostate cancer. Herein, ultrasensitive detection of prostate specific antigen (PSA) aptasensor was realized based on the "on-off-on" model via fluorescence (FL) covalent energy transfer between g-CN quantum dot (g-CNQDs) and palladium triangular plates (Pd TPs). Specifically, the Pd TPs were primarily linked with PSA aptamer (PA) as the reporter probe, followed by attaching them onto the g-CNQDs surfaces, causing the highly enlarged FL quenching rate (ca.
View Article and Find Full Text PDFThe robust and strong electrochemiluminescence (ECL) emission of organic emitters in an aqueous solution is crucial for expanding their applications in early diagnosis. Herein, a Zn porphyrin-based metal-organic framework ((Zn)porphMOF) was facilely obtained by chelating Zn(ii)meso-tetra (4-sulfonatophenyl) porphine (Zn-TSPP) with Zn ions, showing substantially enhanced ECL radiation with KSO as the coreactant via the "reduction-oxidation" route in aqueous media. In contrast with Zn-TSPP, (Zn)porphMOF displayed 22-fold increase in the ECL intensity because of the agglomeration effect.
View Article and Find Full Text PDFNovel and distinct enhancement in electrochemiluminescence (ECL) signals of advanced organic luminophores are of importance for expanding their applications in early diagnosis. This work reported the construction of an ultrasensitive label-free ECL aptasensor for thrombin (TB) detection by grafting zinc proto-porphyrin IX (ZnP) onto an aminated zeolitic imidazole framework-8 (defined as ZnP-NH-ZIF-8 for clarity) as the luminophore. The structure and optical properties of the resulting ZnP-NH-ZIF-8 were carefully characterized.
View Article and Find Full Text PDFA biomimetic assembly of per-O-methylated-cyclodextrin dimer with cobalt proto-porphyrin (Co-PPIX@Py2CD) was achieved via covalent linkage between Co of Co-PPIX and pyridine N of Py2CD (primarily synthesized by the acyl chlorination reaction of two β-CDs monomers with 3,5-bis (bromomethyl) pyridine). Ultraviolet-visible (UV-vis) and circular dichroism (CD) absorption spectroscopy, and NMR hydrogen spectroscopy (H-NMR) were adopted to carefully characterize the structure of Py2CD and its functional assembly with Co-PPIX. X-ray photoelectron spectroscopy (XPS) was employed to affirm the binding of the as-obtained Co-PPIX@Py2CD, whose electrochemical kinetics were extensively studied to validate the feasibility in the catalytic reduction of hydrogen peroxide (HO).
View Article and Find Full Text PDFBy integrating the amplified electrochemical signals and effective capture of antibodies together, advanced multimetallic superstructured nanocrystals endow label-free immunosensors promising applications in early diagnosis and monitoring of diseases. Herein, four-metallic PtCoCuPd hierarchical branch-like tripods (HBTPs) were directly synthesized by a green one-pot aqueous method without any seed or organic solvent involved, which were applied to construct a novel label-free immunosensor for detecting cardiac troponin I (cTnI). The specific hierarchical micro/nanostructures greatly improved the immobilization of antibodies and enhanced the catalytic activity for KFe(CN), which would effectively amplify the electrochemical signals, thereby improving the detection sensitivity.
View Article and Find Full Text PDFA novel sandwich-like immunosensor was efficiently fabricated for detection of carcinoembryonic antigen (CEA) with three dimensional sea-urchin-like PdAuCu nanocrystals (PdAuCu NCs)/ferrocene-grafted-polylysine (Fc-g-PLL) as the label of secondary antibodies (Ab) and Au nanoparticles (Au NPs) as the substrate material. Herein, PdAuCu NCs were directly synthesized with polyethylene oxide (PEO) as a growth-directing agent by a facile one-step aqueous method without any organic solvent. Meanwhile, Fc-g-PLL was obtained by covalent linkage of Fc with PLL via Schiff-base reaction.
View Article and Find Full Text PDFHerein, a novel electrochemical ultrasensitive immunosensor was designed for detecting prostate-specific antigen (PSA) with three-dimensional (3D) PtCu hollow nanoframes (PtCu HNFs) as signal amplification. The highly opened PtCu HNFs were synthesized by a one-pot solvothermal method with cetyltrimethylammonium chloride (CTAC) and trishydroxymethyl aminomethane (Tris) as co-structuring directors. The architectures enlarged the loading of prostate specific antibodies (Ab) and efficiently catalyzed hydrogen peroxide (HO) reaction, ultimately amplifying the signals.
View Article and Find Full Text PDFIt is a main challenge to synthesize highly efficient and durable nanocatalysts towards hydrogen evolution reaction (HER) and alcohol oxidation reaction in energy conversion and storage. Herein, a green wet-chemical approach was developed to directly prepare hollow AgPt nanotube bundles (H-AgPt NTBs), utilizing 5-azacytosine as a structure-directing agent. The obtained electrocatalyst displayed superior catalytic activity and durability for HER in acid media, and the great improvement in catalytic performance for ethylene glycol oxidation reaction (EGOR) in the alkaline electrolyte, outperforming home-made AgPt nanoparticles (NPs), AgPt NPs, and commercial Pt/C catalysts.
View Article and Find Full Text PDFHerein, uniform dendritic PtCo nanoclusters supported on sheet-like polypyrrole (PtCo NCs/PPy) were prepared by a facile one-pot solvothermal method. Cetyltrimethylammonium chloride (CTAC) and pyrrole worked as the capping agent and reductant, respectively, and pyrrole was in-situ polymerized to form PPy sheets under solvothermal conditions. The dendritic PtCo NCs/PPy had the enlarged electrochemically active surface area (EASA, 30.
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