Friedel-Crafts Arylation (the Scholl reaction) is the coupling of two aromatic rings with the aid of a strong Lewis or Brønsted acid. This historically significant C-C bond forming reaction normally leads to aromatic products, often as oligomeric mixtures, dictated by the large stabilization gained upon their rearomatization. The coordination of benzene by a tungsten complex disrupts the natural course of this reaction sequence, allowing for Friedel-Crafts Arylation without rearomatization or oligomerization. Subsequent addition of a nucleophile to the coupled intermediate leads to functionalized cyclohexenes. In this work, we show that by coordinating benzene to tungsten through two carbons (dihapto-coordinate), a rarely observed double protonation of the bound benzene is enabled, allowing its subsequent coupling to a second arene without the need of a precious metal or Lewis acid catalyst.
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http://dx.doi.org/10.1038/s41467-023-38945-0 | DOI Listing |
Spectrochim Acta A Mol Biomol Spectrosc
January 2025
Jilin Key Laboratory of Solid-State Laser Technology and Application, School of Physics, Changchun University of Science and Technology, Changchun 130022 China. Electronic address:
HBT-DPI was a single-molecule multi-conformational fluorescent material and had unique applications for hydrophobic/hydrophilic mapping on large-scale heterogeneous surfaces. In this paper, the different proton transfer processes and luminescence mechanisms of HBT-DPI in Dichloromethane (DCM, no hydrogen bond (HB) receptor) and N, N-Dimethylformamide (DMF, HB receptor) solvents were systematically studied. Using the quantum chemistry method, the stable structures of HBT-DPI in two solvents were determined based on the Boltzmann distribution.
View Article and Find Full Text PDFSci China Life Sci
January 2025
The Key Laboratory of Medical Molecular Cell Biology of Shanxi Province, Institutes of Biomedical Sciences, Shanxi University, Taiyuan, 030006, China.
The cGAS-STING pathway plays a crucial role in the innate immune system by detecting mislocalized double-stranded DNA (dsDNA) in the cytoplasm and triggering downstream signal transduction. Understanding the mechanisms by which cGAS and STING operate is vital for gaining insights into the biology of this pathway. This review provides a detailed examination of the structural features of cGAS and STING proteins, with a particular emphasis on their activation and inhibition mechanisms.
View Article and Find Full Text PDFSci Rep
January 2025
Nonprofitable Organization Touche NPO, Sapporo, 060-004, Japan.
In this study, we explore the structural intricacies of cellulose, a polymer composed of glucose monomers arranged in a linear chain, primarily investigated through solid-state NMR techniques. Specifically, we employ low-field proton nuclear magnetic resonance (H-NMR) to delve into the diverse hydrogen atom types within the cellulose molecule. The low-field H-NMR technique allows us to discern these hydrogen atoms based on their distinct chemical shifts, providing valuable insights into the various functional groups present in cellulose.
View Article and Find Full Text PDFNat Commun
January 2025
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, PR China.
Transition-metal layered double hydroxides are widely utilized as electrocatalysts for the oxygen evolution reaction (OER), undergoing dynamic transformation into active oxyhydroxides during electrochemical operation. Nonetheless, our understanding of the non-equilibrium structural changes that occur during this process remains limited. In this study, utilizing in situ energy-dispersive X-ray absorption spectroscopy and machine learning analysis, we reveal the occurrence of deprotonation and elucidate the role of incorporated iron in facilitating the transition from nickel-iron layered double hydroxide (NiFe LDH) into its active oxyhydroxide.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Division of Chemistry, Graduate School of Science, Kyoto University, Kyoto 606-8502, Japan.
Proton-electron mixed conductors (PEMCs) are an essential component for potential applications in hydrogen separation and energy conversion devices. However, the exploration of PEMCs with excellent mixed conduction, which is quantified by the ambipolar conductivity, σ = σσ/(σ + σ) (σ: electronic conductivity; σ: proton conductivity), is still a great challenge, largely due to the lack of structural characterization of both conducting mechanisms. In this study, we prepared a molecule-based proton-electron mixed-conducting cation radical salt, (ET)[Pt(pop)(Hpop)]·PhCN (ET: bis(ethylenedithio)tetrathiafulvalene, pop: PHO), by electrocrystallization.
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