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Surfactant-Sensitized Covalent Organic Frameworks-Functionalized Lanthanide-Doped Nanocrystals: An Ultrasensitive Sensing Platform for Perfluorooctane Sulfonate.

ABSTRACT: Perfluorooctane sulfonate (PFOS) known as a persistent organic pollutant has been attracting great interests due to its potential ecotoxicity. An approach capable of sensing ultra-trace PFOS is in urgent demand. Here, we developed an approach for highly sensitive sensing PFOS using surfactant-sensitized covalent organic frameworks (COFs)-functionalized upconversion nanoparticles (UCNPs) as a fluorescent probe. COFs-functionalized UCNPs (UCNPs@COFs) were obtained by solvothermal growth of 1,3,5-triformylbenzene and 1,4-phenylenediamine on the surface of UCNPs. COF's layer on the surface of UCNPs not only provides recognition sites for PFOS but also improves the fluorescence quantum yields from 2.15 to 5.12%. Trace PFOS can quench the fluorescence emission of UCNPs@COFs at 550 nm due to the high electronegativity of PFOS. Moreover, the fluorescence quenching response can be significantly strengthened in the presence of a surfactant, which causes more sensitivity. The fluorescence quenching degrees (F ₀ - F) of the system are linear with the concentration of PFOS in the range of 1.8 × 10^-13 to 1.8 × 10^-8 M. The present sensor can sensitively and selectively detect PFOS in tap water and food packing with the limit of detection down to 0.15 pM (signal-to-noise ratio = 3), which is comparable to that of the liquid chromatography-mass spectrometry technique. The proposed approach realized a simple, fast, sensitive, and selective sensing PFOS, showing potential applications in various fields.

SUBMITTER: Li J

PROVIDER: S-EPMC6776982 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Cellulose nanocrystals (CNCs) are biobased colloidal nanorods that have unlocked new opportunities in the area of sustainable functional nanomaterials including structural films and coatings, biomedical devices, energy, sensing, and composite materials. While selective light reflection and sensing develop from the typical chiral nematic (cholesteric, Nem*) liquid crystallinity exhibited by CNCs, a wealth of technologies would benefit from a nematic liquid crystal (LC) with CNC uniaxial alignment. Therefore, this study answers the central question of whether surfactant complexation suppresses CNC chirality in favor of nematic lyotropic and thermotropic liquid crystallinity. Therein, we use a common surfactant having both nonionic and anionic blocks, namely, oligo(ethylene glycol) alkyl-3-sulfopropyl diether potassium salt (an alcohol ethoxy sulfonate (AES)). AES forms complexes with CNCs in toluene (a representative for nonpolar organic solvent) via hydrogen bonding with an AES' oligo(ethylene glycol) block. A sufficiently high AES weight fraction endows the dispersibility of CNC in toluene. Lyotropic liquid crystallinity with Schlieren textures containing two- and four-point brush defects is observed in polarized optical microscopy (POM), along with the suppression of the cholesteric fingerprint textures. The results suggest a nematic (Nem) phase in toluene. Moreover, thermotropic liquid crystallinity is observed by incorporating an excess of AES, in the absence of an additional solvent and upon mild heating. The Schlieren textures suggest a nematic system that undergoes uniaxial alignment under mild shear. Importantly, replacing AES with a corresponding nonionic surfactant does not lead to liquid crystalline properties, suggesting electrostatic structural control of the charged end group of AES. Overall, we introduce a new avenue to suppress CNC chirality to achieve nematic structures, which resolves the long-sought uniaxial alignment of CNCs in filaments, composite materials, and optical devices.

Project description:Perfluorooctane sulfonate (PFOS) has been widely utilized in numerous industries. Due to long environmental and biological half-lives, PFOS is a major public health concern. Although the literature suggests that PFOS may induce neurotoxicity, neurotoxic mechanisms, and neuropathology are poorly understood. Thus, the primary goal of this study was to determine if PFOS is selectively neurotoxic and potentially relevant to specific neurological diseases. Nematodes (Caenorhabditis elegans) were exposed to PFOS or related per- and polyfluoroalkyl substances (PFAS) for 72 h and tested for evidence of neuropathology through examination of cholinergic, dopaminergic, gamma-amino butyric acid (GABA)ergic, and serotoninergic neuronal morphologies. Dopaminergic and cholinergic functional analyses were assessed through 1-nonanol and Aldicarb assay. Mechanistic studies assessed total reactive oxygen species, superoxide ions, and mitochondrial content. Finally, therapeutic approaches were utilized to further examine pathogenic mechanisms. Dopaminergic neuropathology occurred at lower exposure levels (25 ppm, approximately 50 µM) than required to produce neuropathology in GABAergic, serotonergic, and cholinergic neurons (100 ppm, approximately 200 µM). Further, PFOS exposure led to dopamine-dependent functional deficits, without altering acetylcholine-dependent paralysis. Mitochondrial content was affected by PFOS at far lower exposure level than required to induce pathology (≥1 ppm, approximately 2 µM). Perfluorooctane sulfonate exposure also enhanced oxidative stress. Further, mutation in mitochondrial superoxide dismutase rendered animals more vulnerable. Neuroprotective approaches such as antioxidants, PFAS-protein dissociation, and targeted (mitochondrial) radical and electron scavenging were neuroprotective, suggesting specific mechanisms of action. In general, other tested PFAS were less neurotoxic. The primary impact is to prompt research into potential adverse outcomes related to PFAS-induced dopaminergic neurotoxicity in humans.

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Surfactant-Sensitized Covalent Organic Frameworks-Functionalized Lanthanide-Doped Nanocrystals: An Ultrasensitive Sensing Platform for Perfluorooctane Sulfonate.

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