Background: Previous studies indicated that exposure to VOCs was linked to increased systemic inflammation levels. However, the dose-response relationships between urine VOCs metabolites and systemic inflammation have not been established, and the key metabolite of the toxic compounds has not been identified.
Methods: We used data in 7007 US adults in the NHANES cycles (2011-2018) across 8 years.
Previous studies indicated per- and poly-fluoroalkyl substances (PFAS) were related to uric acid and hyperuricemia risk, but evidence for the exposure-response (E-R) curves and combined effect of PFAS mixture is limited. Moreover, the potential mediation effect of kidney function was not assessed. Hence, we conducted a national cross-sectional study involving 13,979 US adults in NHANES 2003-2018 to examine the associations of serum PFAS with uric acid and hyperuricemia risk, and the mediation effects of kidney function.
View Article and Find Full Text PDFAiming at the valuable methylation process, readily available and inexpensive ,,,-tetramethylethylenediamine (TMEDA) was first identified as a new methyl source in photoredox-catalyzed transformation in this work. By virtue of this simple methylating reagent, a facile and practical protocol for the direct C-H methylation of -heteroarenes was developed, featuring mild reaction conditions, broad substrate scope, and scalability. Mechanistic studies disclosed that a sequential photoredox, base-assisted proton shift, fragmentation, and tautomerization process was essentially involved.
View Article and Find Full Text PDFWe herein report an unprecedented photoinduced cyclization/defluorination domino process of -allylbromodifluoroacetamide with cyclic secondary amines. Consequently, a wide array of valuable 3-fluoro-1,5-dihydro-2-pyrrol-2-ones were facilely prepared from readily available starting materials under mild conditions. Preliminary mechanistic investigations suggest that a radical chain propagation and amine-promoted defluorination pathway are presumably involved in this transformation.
View Article and Find Full Text PDFTwo new terragine analogs (‒) with special succinimide and aminopentane moieties were isolated from the fermentation broth of sp. SH-1.2-ROOT-18, an endophyte previously discovered from the root of .
View Article and Find Full Text PDFA visible-light-driven, photocatalyst-free route starting from easily accessed -hydroxycinnamic esters and -perfluoropyridin-4-yl oximes has been successfully developed to rapidly assemble a wide range of 3-cyanoalkyl coumarins. This process does not require addition of external photocatalysts, exhibiting beneficial features including mild reaction conditions, synthetic simplicity, and excellent substrate compatibility. Extensive mechanistic investigations revealed that the in situ generated phenolate anions served as photosensitizers to drive this photoinduced transformation.
View Article and Find Full Text PDFReported herein is the design and synthesis of new -perhalopyridin-4-yl hydroxylamines as shelf-stable and versatile amidyl-radical precursors. The novel amination reagents can be easily prepared via a single synthetic step from inexpensive commercially available starting materials using monoprotected HONH as amino source. The synthetic potency of the developed reagents was well demonstrated by direct amination of a series of quinoxalin-2(1)-ones and their analogues under photocatalytic conditions, even without any additive and photocatalysts.
View Article and Find Full Text PDFA series of functional IRMOF-3 frameworks with solid-state luminescence and tuneable light emission (from 490 to 608 nm) have been synthesized by per-functionalizing AIE-active Schiff-bases with zinc. These precursor AIE-active ligands endowed the functional frameworks with boosted fluorescence emission efficiencies (from 0.16% to 1.
View Article and Find Full Text PDFA visible-light-induced, catalyst-free radical cross-coupling cyclization of diselenides or disulfides with -allylbromodifluoroacetamide has been developed. This developed protocol exhibits good functional group tolerance and affords a variety of 4-thio- and 4-seleno-substituted 3,3-difluoro-γ-lactams in moderate to good yields. Based on control experiments, a plausible radical-radical cross-coupling pathway is proposed.
View Article and Find Full Text PDFThe first photoredox-catalyzed defluoroborylation of polyfluoroarenes with NHC-BH has been facilely achieved at room temperature via a single-electron-transfer (SET)/radical addition pathway. This new strategy makes full use of the advantage of photoredox catalysis to generate the key boryl radical via direct activation of a B-H bond. Good functional group tolerance and high regioselectivity offer this protocol incomparable advantages in preparing a wide array of valuable polyfluoroarylboron compounds.
View Article and Find Full Text PDF-Perfluoropyridin-4-yl group was first installed onto cycloketone oximes as a new electrophore, which was proven to be efficient iminyl radical precursors under photocatalytic and thermal conditions. A range of -perfluoropyridin-4-yl oximes were successfully utilized in C(sp)-C(sp) bond formations of quinoxalin-2(1)-ones and alkenes, providing facile accesses to a range of functionalized alkylnitriles.
View Article and Find Full Text PDFA photoinduced SET process enables the direct B-H bond activation of NHC-boranes. In contrast to common hydrogen atom transfer (HAT) strategies, this photoinduced reaction simply takes advantage of the beneficial redox potentials of NHC-boranes, thus obviating the need for extra radical initiators. The resulting NHC-boryl radical was used for the borylation of a wide range of α-trifluoromethylalkenes and alkenes with diverse electronic and structural features, providing facile access to highly functionalized borylated molecules.
View Article and Find Full Text PDFA photoinduced, phosphoranyl radical-mediated protocol for the direct N-O cleavage of strained cycloketone oximes via a polar/SET crossover process was developed for the first time. This visible-light-driven direct N-O activation mode for oxime offers beneficial features such as streamlined synthetic process and versatile photochemical reactivities. Consequently, the alkenes and α-trifluoromethyl alkenes with varied electronic and structural features acted as competent radical receptors in this protocol, enabling facile accesses to a range of elongated cyano and/or gem-difluoroalkene-bearing compounds.
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