Hydrosilylation of C[double bond, length as m-dash]C double and C[triple bond, length as m-dash]C triple bonds is one of the most widely used processes in organosilicon chemistry, mostly catalyzed by Pt-based complexes. We report here the synthesis of an air-stable dicationic Zn2+-based complex in a hemilabile tris(2-methyl-6-pyridylmethyl) phosphine (TmPPh) ligand, 12+[B(C6F5)4]2. When heated, 12+[B(C6F5)4]2 activates Si-H bonds reversibly via ligand/metal cooperation between Lewis acidic Zn2+ and Lewis basic N centers in a frustrated Lewis pair (FLP) type fashion. Consequently, 12+[B(C6F5)4]2 was found to be an effective catalyst for hydrosilylation reactions of C[double bond, length as m-dash]C double and C[triple bond, length as m-dash]C triple bonds. Remarkably, these hydrosilylation reactions can be loaded under aerobic conditions, as well as, in some cases, work under neat conditions. The mechanism of the activation of the Si-H bond and the hydrosilylation reaction is proposed based on experiments and density functional theory (DFT) calculations.
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RSC Adv
January 2025
Gansu Zhongshang Food Quality Test and Detection Co., Ltd Lanzhou 730010 China.
Ferrihydrite (Fh), a widely distributed mineral in the environment, plays a crucial role in the geochemical cycling of elements. This study used experimental and computational approaches to investigate the adsorption behavior of seven heavy metal ions on Fh. The pH edge analysis revealed that the adsorption capacity followed the order: Pb > Cu > Zn > Cd > Ni > Co > Mn, with Pb showed the highest adsorption.
View Article and Find Full Text PDFNoncovalent carbon bonding (C-bonding), a recently explored σ-hole interaction, has primarily been characterized through X-ray structural and computational studies. Evidence of C-bonds in solution is scarce, especially in highly polar solvents like DMSO where solvation effects typically overshadow weak non-covalent interactions. In this work, we present three novel spiroisatin-based -acyl hydrazones (1-3) in which C-bonds play a critical role in stabilizing the conformation in solution.
View Article and Find Full Text PDFEnviron Sci Technol
January 2025
State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550081, PR China.
Cadmium (Cd) isotopes have recently emerged as novel tracers of Cd sources and geochemical processes. Widespread clay minerals play a key role in Cd migration due to their strong adsorption capacity, but the mechanism of Cd isotope fractionation during adsorption onto clay minerals is poorly understood. Here, we experimentally investigated the adsorption mechanisms of Cd on montmorillonite (2:1) and kaolinite (1:1) by using extended X-ray absorption fine structure (EXAFS) spectroscopy.
View Article and Find Full Text PDFNanotechnology
January 2025
Department of Electrical and Computer Engineering, Nazarbayev University, Nazarbayev University, Astana, Kazakhstan, Astana, 010000, KAZAKHSTAN.
Non-equilibrium molecular dynamics (NEMD) simulations reveal the existence of a spontaneous heat current (SHC) in the absence of a temperature gradient and demonstrate ultra-high thermal rectification in asymmetric trapezoid-shaped graphene. These unique properties have potential applications in power generation and thermal circuits, functioning as thermal diodes. Our findings also show the presence of negative and zero thermal conductivity in this system.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, P. R. China.
The microenvironment is recognized to be as crucial as active sites in heterogeneous catalysis. It was found that the catalytic activity of a set of chemical reactions can be significantly influenced by the confined space of carbon nanotubes (CNTs), with some reactions showing superior activity, while others experience a negative impact. The rational design of confined catalysis must rely on the accurate insights of confined microenvironment.
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