Pt nanoparticles entrapped in ordered mesoporous CMK-3 carbons with p6mm symmetry were prepared using a facile impregnation method, and the resulting materials were characterized using X-ray diffraction spectroscopy, ...Pt nanoparticles entrapped in ordered mesoporous CMK-3 carbons with p6mm symmetry were prepared using a facile impregnation method, and the resulting materials were characterized using X-ray diffraction spectroscopy, N2 adsorption-desorption, scanning electron microscopy, transmission electron microscopy, energy dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. The Pt nanoparticles were highly dispersed in the CMK-3 with 43.7% dispersion. The Pt/CMK-3 catalyst was an effective catalyst for the liquid-phase hydrogenation of nitrobenzene and its derivatives under the experimental conditions studied here. The Pt/CMK-3 catalyst was more active than commercial Pt/C catalyst in most cases. A highest turnover frequency of 43.8 s-1 was measured when the Pt/CMK-3 catalyst was applied for the hydrogenation of 2-methyl-nitrobenzene in ethanol under optimal conditions. It is worthy of note that the Pt/CMK-3 catalyst could be recycled easily, and could be reused at least fourteen times without any loss in activity or selectivity for the hydrogenation of nitrobenzene in ethanol.展开更多
Facile synthetic approaches toward the development of efficient and durable nonprecious metal catalysts for the oxygen reduction reaction (ORR) are very important for commercializing advanced electrochemical devices...Facile synthetic approaches toward the development of efficient and durable nonprecious metal catalysts for the oxygen reduction reaction (ORR) are very important for commercializing advanced electrochemical devices such as fuel cells and metal-air batteries. Here we report a novel template approach to synthesize mesoporous Fe-N-doped carbon catalysts encapsulated with Fe3C nanoparticles. In this approach, the layer-structured FeOCI was first used as a template for the synthesis of a three- dimensional polypyrrole (PPy) structure. During the removal of the FeOCI template, the Fe^3+ can be absorbed by PPy and then converted into Fe3C nanoparticles and Fe-N-C sites during the pyrolyzing process. As a result, the as-prepared catalysts could exhibit superior electrocatalytic ORR performance to the commercial Pt/C catalyst in alkaline solutions. Furthermore, the Zn-air battery assembled using the mesoporous carbon catalyst as the air electrode could surpass the commercial Pt/C catalyst in terms of the power density and energy density.展开更多
Controllable fabrication of mesoporous carbon nanoparticles(MCNs)with tunable pore structures is of great interest,due to the remarkable effect of pore structure on electrochemical performance of the materials.However...Controllable fabrication of mesoporous carbon nanoparticles(MCNs)with tunable pore structures is of great interest,due to the remarkable effect of pore structure on electrochemical performance of the materials.However,it has remained a major challenge.Here,we demonstrate the controlled synthesis of MCNs with tunable closed pore structures via a silica-assisted coassembly strategy,which employs polystyrene-block-poly(ethylene oxide)diblock copolymers as soft template,phenolic resol and tetraethyl orthosilicate as carbon and silica precursors,respectively.Through simply varying the sequential cross-linking of the silica and carbon precursors or the copolymer composition,novel MCNs with alluring spherical,hollow-hoop-structured,or yolk-shell-like closed mesopores are tunably prepared.In particular,serving as cathode materials of lithium-sulfur batteries,the resultant silica-hybridized MCNs with the exceptional hollow-hoop mesopores and a moderate sulfur-loading content of 46 wt%exhibit top-level electrochemical performance.This study opens an avenue for tunable construction of mesoporous particles with closed pores and provides clues for the effect of pore geometry on the electrochemical performance of porous cathode materials for lithium-sulfur batteries.展开更多
基金supported by the National Natural Science Foundation of China(21273076 and 21373089)the Open Research Fund of Top Key Discipline of Chemistry in Zhejiang Provincial Colleges and Key Laboratory of the Ministry of Education for Catalysis Materials(Zhejiang Normal University,ZJHX2013)Shanghai Leading Academic Discipline Project (B409)~~
文摘Pt nanoparticles entrapped in ordered mesoporous CMK-3 carbons with p6mm symmetry were prepared using a facile impregnation method, and the resulting materials were characterized using X-ray diffraction spectroscopy, N2 adsorption-desorption, scanning electron microscopy, transmission electron microscopy, energy dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. The Pt nanoparticles were highly dispersed in the CMK-3 with 43.7% dispersion. The Pt/CMK-3 catalyst was an effective catalyst for the liquid-phase hydrogenation of nitrobenzene and its derivatives under the experimental conditions studied here. The Pt/CMK-3 catalyst was more active than commercial Pt/C catalyst in most cases. A highest turnover frequency of 43.8 s-1 was measured when the Pt/CMK-3 catalyst was applied for the hydrogenation of 2-methyl-nitrobenzene in ethanol under optimal conditions. It is worthy of note that the Pt/CMK-3 catalyst could be recycled easily, and could be reused at least fourteen times without any loss in activity or selectivity for the hydrogenation of nitrobenzene in ethanol.
基金supported by the National Key Basic Research Program of China (No. 2015CB351903)National Natural Science Foundation of China (No. 51402282)+1 种基金China Postdoctoral Science Foundation (No. 2016M590579)the Fundamental Research Funds for the Central Universities
文摘Facile synthetic approaches toward the development of efficient and durable nonprecious metal catalysts for the oxygen reduction reaction (ORR) are very important for commercializing advanced electrochemical devices such as fuel cells and metal-air batteries. Here we report a novel template approach to synthesize mesoporous Fe-N-doped carbon catalysts encapsulated with Fe3C nanoparticles. In this approach, the layer-structured FeOCI was first used as a template for the synthesis of a three- dimensional polypyrrole (PPy) structure. During the removal of the FeOCI template, the Fe^3+ can be absorbed by PPy and then converted into Fe3C nanoparticles and Fe-N-C sites during the pyrolyzing process. As a result, the as-prepared catalysts could exhibit superior electrocatalytic ORR performance to the commercial Pt/C catalyst in alkaline solutions. Furthermore, the Zn-air battery assembled using the mesoporous carbon catalyst as the air electrode could surpass the commercial Pt/C catalyst in terms of the power density and energy density.
基金This work was supported by the National Natural Science Foundation of China(nos.21774076,61774102,and 51573091)the National Key Research and Development Program of China(no.2017YFE0195800)+2 种基金the Program of the Shanghai Committee of Science and Technology(no.17JC1403200)the Program of Shanghai Academic Research Leader(no.19XD1421700)the Program of Shanghai Eastern Scholar.
文摘Controllable fabrication of mesoporous carbon nanoparticles(MCNs)with tunable pore structures is of great interest,due to the remarkable effect of pore structure on electrochemical performance of the materials.However,it has remained a major challenge.Here,we demonstrate the controlled synthesis of MCNs with tunable closed pore structures via a silica-assisted coassembly strategy,which employs polystyrene-block-poly(ethylene oxide)diblock copolymers as soft template,phenolic resol and tetraethyl orthosilicate as carbon and silica precursors,respectively.Through simply varying the sequential cross-linking of the silica and carbon precursors or the copolymer composition,novel MCNs with alluring spherical,hollow-hoop-structured,or yolk-shell-like closed mesopores are tunably prepared.In particular,serving as cathode materials of lithium-sulfur batteries,the resultant silica-hybridized MCNs with the exceptional hollow-hoop mesopores and a moderate sulfur-loading content of 46 wt%exhibit top-level electrochemical performance.This study opens an avenue for tunable construction of mesoporous particles with closed pores and provides clues for the effect of pore geometry on the electrochemical performance of porous cathode materials for lithium-sulfur batteries.