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131.
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
132.
Philip J. Hammond C. Dennis Hall 《Phosphorus, sulfur, and silicon and the related elements》2013,188(3):351-353
Abstract Cis-1-alkyl (or aryl)-2,5-dimethyl-3-phospholens isomerize to the trans-isomers in deuteriochloroform and the isomerization is probably due to small quantities of phosgene in the solvent. 相似文献
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135.
Dr. Xiong‐Jie Jiang Dr. Janet T. F. Lau Dr. Qiong Wang Prof. Dennis K. P. Ng Prof. Pui‐Chi Lo 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(24):8273-8281
A diiodo distyryl boron dipyrromethene (BODIPY) core was conjugated to two ferrocenyl quenchers through acid‐labile ketal and/or thiol‐cleavable disulfide linkers, of which the fluorescence and photosensitizing properties were significantly quenched through a photoinduced electron‐transfer process. The two symmetrical analogues that contained either the ketal or disulfide linkers could only be activated by a single stimulus, whereas the unsymmetrical analogue was responsive to dual stimuli. Upon interaction with acid and/or dithiothreitol (DTT), these linkers were cleaved selectively. The separation of the BODIPY core and the ferrocenyl moieties restored the photoactivities of the former in phosphate buffered saline and inside the MCF‐7 breast cancer cells, rendering these compounds as potential activable photosensitizers for targeted photodynamic therapy. The dual activable analogue exhibited the greatest enhancement in intracellular fluorescence intensity in both an acidic environment (pH 5) and the presence of DTT (4 mm ). Its photocytotoxicity against MCF‐7 cells also increased by about twofold upon preincubation with 4 mm of DTT. The activation of this compound was also demonstrated in nude mice bearing a HT29 human colorectal carcinoma. A significant increase in fluorescence intensity in the tumor was observed over 9 h after intratumoral injection. 相似文献
136.
Jiang Yuan Jinming Duan Wei Li Christopher P. Saint Dennis Mulcahy 《Chromatographia》2017,80(2):247-257
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138.
Han Joong Koh Suk Jin Kang Dennis N. Kevill 《Phosphorus, sulfur, and silicon and the related elements》2013,188(7):1404-1415
Kinetic and product studies of the solvolyses of acyclic phosphorochloridates are extended to two cyclic diesters, 2-chloro-1,3,2-dioxaphospholane-2-oxide (1) and 2-chloro-5,5-dimethyl-1,3,2-dioxaphosphorinane-2-oxide (2). Slightly faster solvolyses are observed for 1 than for the acyclic dimethyl phosphorochloridate (3), and 2 solvolyzes somewhat slower than 3. An extended Grunwald–Winstein equation treatment shows similar sensitivities to changes in solvent nucleophilicity and solvent ionizing power for 1, 2, and 3, and a concerted SN2 attack is proposed in each case. Product studies for the solvolyses of 2 in aqueous alcohols are presented. 相似文献
139.
Martin Pomerantz Jiping Wang Seeyearl Seong Kyle P. Starkey Long Nguyen Dennis S. Marynick 《Phosphorus, sulfur, and silicon and the related elements》2013,188(1-4):507-508
Abstract Poly(benzo[1,2-b:4,5-b′]dithiophene-4,8-diyl vinylene) (1) has been prepared by the pyrolysis of the precursor polymer 2 and studied. Quantum mechanical calculations on the aromatic and quinoid monomers, oligomers and polymers indicate that 1 is a planar aromatic polymer. 相似文献
140.
Hendrik F. Hameka Silvio L. Emery George R. Famini James O. Jensen Joseph M. Leonard Dennis J. Reutter 《Phosphorus, sulfur, and silicon and the related elements》2013,188(1-4):373-388
Abstract We report the computed equilibrium geometries and vibrational infrared frequencies of a group of thirteen mercaptans and sulfides. The computations were based on the Gaussian 86 Program Package utilizing 3-21G basis sets. The theoretical bond distances and bond angles are in agreement with the available experimental data. The agreement between computed frequencies and available experimental values seems reasonable. We also used the computations as guidelines for the assignment of available experimental infrared frequencies. We believe that it is possible to make reliable frequency predictions by combining computations with available experimental data for groups of similar molecules. However, it is necessary to introduce different correction factors for different types of vibrational modes if we use 3-21G basis sets. 相似文献