Nitrogen‐doped polycyclic aromatic hydrocarbons (aza‐PAHs) have found broad applications in material sciences. Herein, a modular electrochemical synthesis of aza‐PAHs was developed via a rhodium‐catalyzed cascade C−H activation and alkyne annulation. A multifunctional O‐methylamidoxime enabled the high chemo‐ and regioselectivity. The isolation of two key rhodacyclic intermediates made it possible to delineate the exact order of three C−H activation steps. In addition, the metalla‐electrocatalyzed multiple C−H transformation is characterized by unique functional group tolerance, including highly reactive iodo and azido groups.
N, P and SiO3-Si in the Changjiang mainstream and its major tributaries and lakes were investigated in the dry season from November to December, 1997, and in the flood season in August and October, 1998. An even distribution of SiO3-Si was found along the Changjiang River. However, the concentrations of total nitrogen, total dissolved nitrogen, dissolved inorganic nitrogen, nitrate and total phosphorus, total particulate phosphorus increased notably in the upper reaches, which reflected an increasing impact from human activities. Those concentrations in the middle and lower reaches of the Changjiang River were relatively constant. Dissolved N was the major form of N and the particulate P was the major form of P in the Changjiang River. The molar ratio of dissolved N to dissolved P was extremely high (192.5-317.5), while that of the particulate form was low (5.6-37.7). High N/P ratio reflected a significant input of anthropogenic N such as N from precipitation and N lost from water and soil etc. Dissolved N and P was in a quasi-equilibrium state in the process from precipitate to the river. In the turbid river water, light limitation, rather than P limitation, seemed more likely to be a controlling factor for the growth of phytoplankton. A positive linear correlationship between the concentration of dissolved N and the river's runoff was found, mainly in the upper reaches, which was related to the non-point sources of N. Over the past decades, N concentration has greatly increased, but the change of P concentration was not as significant as N. The nutrient fluxes of the Changjiang mainstream and tributaries were estimated, and the result showed that the nutrient fluxes were mainly controlled by the runoff, of which more than a half came from the tributaries. These investigations carried out before water storage of the Three Gorges Dam will supply a scientific base for studying the influences of the Three Gorges Dam on the ecology and environment of the Changjiang River and its estuary.
We describe the self-assembly of gold nanoparticles (Au NPs) protected with newly synthesized discotic liquid crystalline molecules of hexaalkoxy-substituted triphenylene (TP) in mixed toluene/methanol solvent. The stripelike (i.e., 2D consisting of linear 1D in stripe) self-assembly is realized successfully by the aid of pi-pi stacking of TP ligand on Au NPs. The smaller Au NPs with TP (AuTP) or the longer alkyl chain between TP and the gold core provide more free spaces among TP moieties. These spaces allow easy insertion of TP on adjacent AuTPs to lead an interparticle pi-pi interaction to form the stripelike arrangement. The solvent hydrophilicity can also serve as a controlled index to tune arrangement among stripelike, hexagonal close packed (hcp), or disorder. We have changed the solvent hydrophilicity by changing the ratio of methanol to toluene, which affects the balance of solution of AuTP (in toluene) and deposition (in methanol). The larger space between TPs and appropriate solvent hydrophilicity realize stripelike self-assembly caused by a strong pi-pi interaction between TPs, which was characterized by TEM, as well as fluorescence, dynamic light scattering, and 1H NMR spectra.
C-H alkylations with challenging β-hydrogen-containing alkyl halides were accomplished with sustainable MnCl as the catalyst under phosphine-ligand-free conditions. The proximity-induced benzamide C-H activation occurred with ample substrate scope through rate-determining C-H metalation, also setting the stage for manganese-catalyzed oxidative C-H methylations.
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