Cu2O and Cul were supported on multiwalled carbon nanotubes （MWCNTs） using a wet impregna- tion method, and the resulting materials were fully characterized by powder X-ray diffraction, Fourier transform infrared sp...Cu2O and Cul were supported on multiwalled carbon nanotubes （MWCNTs） using a wet impregna- tion method, and the resulting materials were fully characterized by powder X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy with energy dispersive X-ray spectroscopy, transmission electron microscopy, and temperature-programmed desorption with ammonia analysis. The results of these experiments revealed that Cu2O and CuI were deposited on the MWCNTs in the cubic and γ phases, respectively. These results also showed that the Cu-containing MWCNTs exhibited weak to strong electron-accepting （Lewis acidic） properties. The catalytic activities of these materials were studied for the synthesis of biologically significant N-（pyridin-2-yl）benzamides via the oxidative amidation of aryl aldehydes with 2-aminopyridines. The yields of the products were in the range 50%-95% with 100% selectivity. Notably, the CuI/MWCNT catalyst was much more effective than the Cu2O/MWCNT catalyst with respect to the isolated yield of the product, although the latter of these two catalysts exhibited much better recyclability. A preferential interaction was observed between the polar nature of the acid-activated MWCNTs and the ionic Cu2O compared with covalent CuL The differences in these interactions had a significant impact on the rate of the nucleophilic attack of the amino group of 2-aminopyridine substrate on the carbonyl group of the aryl aldehyde.展开更多
A facile design of Pt nanostructures from submonolayer to monolayer has been realized by ion adsorption-in situ electrochemical reduction on Au nanoparticles supported on multiwall carbon nanotubes （CNTs）. The as pr...A facile design of Pt nanostructures from submonolayer to monolayer has been realized by ion adsorption-in situ electrochemical reduction on Au nanoparticles supported on multiwall carbon nanotubes （CNTs）. The as prepared Au@Pt/CNTs catalysts display coverage-specific electrocatalysis. Au@Pt/CNTs with low Pt coverage is inactive towards methanol oxidation whereas it oxidizes formic acid effectively through a direct pathway with mass specific activity 90 times that of a commercial Pt/C catalyst. Due to its inertness to methanol, it shows high performance in the oxygen reduction reaction （ORR） with high methanol tolerance. In contrast, simply increasing the Pt coverage to above 40% switches the formic acid oxidation process to both direct and indirect catalytic pathways, and also results in high methanol oxidation activity.展开更多
Based on the noncovalent functionalization of ferrocene-grafted polyethylenimine （PEI-Fc） and carbon nanotubes （CNTs）, CNT bundles are exfoliated by PEI-Fc solution and thus form stable compounds PEI-Fc@CNTs, whic...Based on the noncovalent functionalization of ferrocene-grafted polyethylenimine （PEI-Fc） and carbon nanotubes （CNTs）, CNT bundles are exfoliated by PEI-Fc solution and thus form stable compounds PEI-Fc@CNTs, which is used to construct the PEI-Fc@CNTs/DNA multilayers through layer-by-layer assembly. The multilayers show a highly uniform and homogeneous characteristic, which significantly improve the electrical property of the multilayers. Upon the oxidation electrical potential, the ferrocene groups are switched from reduction state （[Fe（C5H5）2]） to oxidation state （[Fe（C5H5）2]^＋）, leading to change of microenvironments＇ charge density, resulting in swelling of the multilayers and a final degree of swelling of 37 % and the decrease of multilayer stiffness. We maintain that electrochemical control over the swelling behavior of multilayers could have important implications for responsive coatings of nanoscale devices, including mechanically tunable surfaces which are used to modulate cellular activities and control drug delivery.展开更多
基金DST-SERB for the financial support for this research work(Project number:SERB/F/3690/2013-14)
文摘Cu2O and Cul were supported on multiwalled carbon nanotubes （MWCNTs） using a wet impregna- tion method, and the resulting materials were fully characterized by powder X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy with energy dispersive X-ray spectroscopy, transmission electron microscopy, and temperature-programmed desorption with ammonia analysis. The results of these experiments revealed that Cu2O and CuI were deposited on the MWCNTs in the cubic and γ phases, respectively. These results also showed that the Cu-containing MWCNTs exhibited weak to strong electron-accepting （Lewis acidic） properties. The catalytic activities of these materials were studied for the synthesis of biologically significant N-（pyridin-2-yl）benzamides via the oxidative amidation of aryl aldehydes with 2-aminopyridines. The yields of the products were in the range 50%-95% with 100% selectivity. Notably, the CuI/MWCNT catalyst was much more effective than the Cu2O/MWCNT catalyst with respect to the isolated yield of the product, although the latter of these two catalysts exhibited much better recyclability. A preferential interaction was observed between the polar nature of the acid-activated MWCNTs and the ionic Cu2O compared with covalent CuL The differences in these interactions had a significant impact on the rate of the nucleophilic attack of the amino group of 2-aminopyridine substrate on the carbonyl group of the aryl aldehyde.
文摘A facile design of Pt nanostructures from submonolayer to monolayer has been realized by ion adsorption-in situ electrochemical reduction on Au nanoparticles supported on multiwall carbon nanotubes （CNTs）. The as prepared Au@Pt/CNTs catalysts display coverage-specific electrocatalysis. Au@Pt/CNTs with low Pt coverage is inactive towards methanol oxidation whereas it oxidizes formic acid effectively through a direct pathway with mass specific activity 90 times that of a commercial Pt/C catalyst. Due to its inertness to methanol, it shows high performance in the oxygen reduction reaction （ORR） with high methanol tolerance. In contrast, simply increasing the Pt coverage to above 40% switches the formic acid oxidation process to both direct and indirect catalytic pathways, and also results in high methanol oxidation activity.
基金supported by the National Natural Science Foundation of China(21174126,51333005,21374095)the National Basic Research Program of China(2011CB606203)+2 种基金Research Fund for the Doctoral Program of Higher Education of China(20110101110037,20120101130013)the Qianjiang Excellence Project of Zhejiang Province(2013R10035)International Science&Technology Cooperation Program of China(2014DFG52320)
文摘Based on the noncovalent functionalization of ferrocene-grafted polyethylenimine （PEI-Fc） and carbon nanotubes （CNTs）, CNT bundles are exfoliated by PEI-Fc solution and thus form stable compounds PEI-Fc@CNTs, which is used to construct the PEI-Fc@CNTs/DNA multilayers through layer-by-layer assembly. The multilayers show a highly uniform and homogeneous characteristic, which significantly improve the electrical property of the multilayers. Upon the oxidation electrical potential, the ferrocene groups are switched from reduction state （[Fe（C5H5）2]） to oxidation state （[Fe（C5H5）2]^＋）, leading to change of microenvironments＇ charge density, resulting in swelling of the multilayers and a final degree of swelling of 37 % and the decrease of multilayer stiffness. We maintain that electrochemical control over the swelling behavior of multilayers could have important implications for responsive coatings of nanoscale devices, including mechanically tunable surfaces which are used to modulate cellular activities and control drug delivery.
