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121.
David M. Koshy Dr. Shucheng Chen Dr. Dong Un Lee Dr. Michaela Burke Stevens Ahmed M. Abdellah Samuel M. Dull Gan Chen Dr. Dennis Nordlund Dr. Alessandro Gallo Dr. Christopher Hahn Dr. Drew C. Higgins Dr. Zhenan Bao Dr. Thomas F. Jaramillo 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(10):4072-4079
Ni,N-doped carbon catalysts have shown promising catalytic performance for CO2 electroreduction (CO2R) to CO; this activity has often been attributed to the presence of nitrogen-coordinated, single Ni atom active sites. However, experimentally confirming Ni−N bonding and correlating CO2 reduction (CO2R) activity to these species has remained a fundamental challenge. We synthesized polyacrylonitrile-derived Ni,N-doped carbon electrocatalysts (Ni-PACN) with a range of pyrolysis temperatures and Ni loadings and correlated their electrochemical activity with extensive physiochemical characterization to rigorously address the origin of activity in these materials. We found that the CO2R to CO partial current density increased with increased Ni content before plateauing at 2 wt % which suggests a dispersed Ni active site. These dispersed active sites were investigated by hard and soft X-ray spectroscopy, which revealed that pyrrolic nitrogen ligands selectively bind Ni atoms in a distorted square-planar geometry that strongly resembles the active sites of molecular metal–porphyrin catalysts. 相似文献
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124.
Solène Morand Prof. Philippe Jubault Prof. Jean-Philippe Bouillon Dr. Samuel Couve-Bonnaire 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(69):17273-17292
gem-Heteroatom-substituted fluoroalkenes have received little attention despite their great potential in medicinal chemistry or in fine chemistry. Indeed, due to the electronic and steric similarity between the fluoroalkene moiety and the amide bond as well as the high strength of the carbon-fluorine bond, these gem-heteroatom-substituted fluoroalkenes could be envisioned as stable mimics of various important organic functions, such as phosphates, carbamates, S-thiocarbamates and ureas. We present herein an overview describing the syntheses over the last decade of heteroatom-substituted fluoroalkenes in geminal position. This review will be divided into several sections covering each the common following heteroatom: oxygen-, nitrogen-, sulfur-, phosphorus-, boron- and silicon-substituted fluoroalkenes. 相似文献
125.
A trigonometrically fitted block Numerov type method (TBNM), is proposed for solving y′′?=?f(x, y, y′) directly without reducing it to an equivalent first order system. This is achieved by constructing a continuous representation of the trigonometrically fitted Numerov method (CTNM) and using it to generate the well known trigonometrically fitted Numerov method (TNUM) and three new additional methods, which are combined and applied in block form as simultaneous numerical integrators. The stability property of the TBNM is discussed and the performance of the method is demonstrated on some numerical examples to show accuracy and efficiency advantages. 相似文献
126.
Felipe Wodtke Fernando R. Xavier Samuel R. Mendes Alfredo R.M. de Oliveira Rogério A. Gariani 《Tetrahedron letters》2017,58(3):231-234
A novel application of the highly stable niobium oxide phosphate (NbOPO4) as an efficient catalyst for the synthesis of β-enamino ketones under solvent-free conditions is described. This protocol, exhibits attractive yields, short reaction periods, lower loading of catalyst and high chemoselectivity. 相似文献
127.
Claudio C. Silveira Samuel R. Mendes Guilherme M. Martins 《Tetrahedron letters》2012,53(13):1567-1570
Ce(OTf)3 was successfully employed as catalyst for the activation of the hydroxyl group in the Friedel–Crafts reaction of aromatic compounds with propargylic alcohols in nitromethane. The products were obtained in good to excellent yields. 相似文献
128.
Samuel O. Grim Anthony W. Yankowsky 《Phosphorus, sulfur, and silicon and the related elements》2013,188(2):191-195
Abstract The 31P chemical shifts of eleven (4-ZC6H4)3P compounds show a slight correlation with the Hammet [sgrave]para constant of Z. The unusually large upfield chemical shifts of (2-ZC6H4)3P compounds are attributed to an extreme “gamma” effect caused by the restricted conformations due to the steric influence of the ortho substituents. Chemical shifts are given for about thirty triarylphosphines, and group contributions to phosphine chemical shifts are listed for twenty-one aryl groups. 相似文献
129.
Samuel O. Grim Mudlagiri B. Goli 《Phosphorus, sulfur, and silicon and the related elements》2013,188(3-4)
Abstract 1,1-Bis(diphenylphosphino)ethene, 1a, was originally prepared by Colquhoun and McFarlane1 by the reaction of lithium diphenylphosphide and vinylidene chloride. Subsequently, Schmidbaur et al.,2 reported further novel chemistry of 1a and its derivatives such as 1b and 1c. 相似文献
130.