The heterogeneously copper-catalyzed oxidative cleavage of styrene was studied using copper-doped mesoporous KIT-6(CU-KIT-6_x) prepared via pH adjustment(where x is the pH:1.43,2.27,3.78,3.97,4.24 or 6.62).Variat...The heterogeneously copper-catalyzed oxidative cleavage of styrene was studied using copper-doped mesoporous KIT-6(CU-KIT-6_x) prepared via pH adjustment(where x is the pH:1.43,2.27,3.78,3.97,4.24 or 6.62).Variations in the catalyst structure and morphology with pH values were characterized by X-ray power diffraction,nitrogen adsorption-desorption analysis,transmission electron microscopy and X-ray photoelectron spectroscopy.As the pH value applied during the initial synthesis,the resulting Cu-KIT-6_x exhibited different structural,textural and surface characteristics,especially in terms of specific copper species and copper content At a pH value of 3.78,approximately 4.6 wt%copper(Ⅱ) was successfully incorporated into the framework of the initial KIT-6,in the form of-Cu-O-Si- groups.The catalytic performance of each catalyst was evaluated by following the epoxidation of styrene,employing tert-butyl hydroperoxide as the oxidant and CH_3CN as the solvent.A significant styrene conversion of 43.5%with 86.6%selectivity for the desired styrene epoxide was obtained over the Cu-KIT-63.78.A higher Cu content,an ordered cubic laid mesoporous architecture and various specific textural characteristics all combined to endow the Cu-KIT-63.78 with high catalytic activity and good stability.展开更多
Spinel LiMn2O4 microspheres with durable high rate capability were synthesized by a facile route using spherical MnCO3 precursors as the self-supported templates, combined with the calcinations of LiNO3 at 700 °C...Spinel LiMn2O4 microspheres with durable high rate capability were synthesized by a facile route using spherical MnCO3 precursors as the self-supported templates, combined with the calcinations of LiNO3 at 700 °C for 8 h. The spherical MnCO3 precursors were obtained from the control of the crystallizing process of Mn2+ ions and NH4HCO3 in aqueous solution. The effects of the mole ratio of the raw materials, reaction time, and reaction temperature on the morphology and yield of the MnCO3 were investigated. The as-synthesized MnCO3 and LiMn2O4 microspheres were characterized by powder X-ray diffractometry (XRD) and scanning electron microscopy (SEM). Galvanostatic charge/discharge tests indicate that the spinel LiMn2O4 microspheres deliver a discharge capacity of 90 mA-h/g at 10C rate show good capacity retention capability (75% of their initial capacity after 800 cycles at 10C rate). The durable high rate capability suggests that the as-synthesized LiMn2O4 microspheres are promising cathode materials for high power lithium ion batteries.展开更多
Metal-organic-framework (MOF)-based materials with novel physicochemical properties have emerged as promising catalysts for various hydrogenation reactions. In addition to metal clusters and multifunctional organic...Metal-organic-framework (MOF)-based materials with novel physicochemical properties have emerged as promising catalysts for various hydrogenation reactions. In addition to metal clusters and multifunctional organic ligands, MOF-based catalysts can incorporate other functional species, and thus provide various active sites for hydrogenation processes. The structural properties of the catalysts play significant roles in enhancing the interactions among the reactants, products, and catalytic sites, which can be rationally designed. Because of the synergistic effects between the ac-tive sites and the structural properties, MOF-based catalysts can achieve higher activities and selec- tivities in hydrogenation reactions than can be obtained using traditional heterogeneous catalysts. This review provides an overview of recent developments in MOF-based catalysts in the hydro-genation of alkenes, alkynes, nitroarenes, cinnamaldehyde, furfural, benzene, and other compounds. Strategies for improving the catalytic performances of MOF-based catalysts are discussed as well as the different active sites and structural properties of the catalysts.展开更多
基金supported by Guangdong Science and Technology Planning Project(2015A020216002)Guangdong Natural Science Foundation(2014A030313259)the National Natural Science Foundation of China(21543014,21173086,U1301245)~~
文摘The heterogeneously copper-catalyzed oxidative cleavage of styrene was studied using copper-doped mesoporous KIT-6(CU-KIT-6_x) prepared via pH adjustment(where x is the pH:1.43,2.27,3.78,3.97,4.24 or 6.62).Variations in the catalyst structure and morphology with pH values were characterized by X-ray power diffraction,nitrogen adsorption-desorption analysis,transmission electron microscopy and X-ray photoelectron spectroscopy.As the pH value applied during the initial synthesis,the resulting Cu-KIT-6_x exhibited different structural,textural and surface characteristics,especially in terms of specific copper species and copper content At a pH value of 3.78,approximately 4.6 wt%copper(Ⅱ) was successfully incorporated into the framework of the initial KIT-6,in the form of-Cu-O-Si- groups.The catalytic performance of each catalyst was evaluated by following the epoxidation of styrene,employing tert-butyl hydroperoxide as the oxidant and CH_3CN as the solvent.A significant styrene conversion of 43.5%with 86.6%selectivity for the desired styrene epoxide was obtained over the Cu-KIT-63.78.A higher Cu content,an ordered cubic laid mesoporous architecture and various specific textural characteristics all combined to endow the Cu-KIT-63.78 with high catalytic activity and good stability.
基金supported by the National Natural Science Foundation of China(21476087)Pearl River S&T Nova Program of Guangzhou(2013J2200041)+2 种基金the Science & Technology Research Project of Guangdong Province(2014A010105041)Guangdong Natural Science Foundation(S2013010012469)Innovation Project of Guangdong Department of Education(2014KTSCX016)~~
基金Project(2011M501090) upported by the China Postdoctoral Science FoundationProject(SCUT2012ZZ0042) upported by the Fundamental Research Funds for the Central Universities+1 种基金Project supported by the"SPR-2011"of South China University of TechnologyProject(NRC07/08.EG01)supprted by the Fok Ying Tung Foundation
文摘Spinel LiMn2O4 microspheres with durable high rate capability were synthesized by a facile route using spherical MnCO3 precursors as the self-supported templates, combined with the calcinations of LiNO3 at 700 °C for 8 h. The spherical MnCO3 precursors were obtained from the control of the crystallizing process of Mn2+ ions and NH4HCO3 in aqueous solution. The effects of the mole ratio of the raw materials, reaction time, and reaction temperature on the morphology and yield of the MnCO3 were investigated. The as-synthesized MnCO3 and LiMn2O4 microspheres were characterized by powder X-ray diffractometry (XRD) and scanning electron microscopy (SEM). Galvanostatic charge/discharge tests indicate that the spinel LiMn2O4 microspheres deliver a discharge capacity of 90 mA-h/g at 10C rate show good capacity retention capability (75% of their initial capacity after 800 cycles at 10C rate). The durable high rate capability suggests that the as-synthesized LiMn2O4 microspheres are promising cathode materials for high power lithium ion batteries.
基金supported by the National Natural Science Foundation of China(21322606,21436005,21576095)China Postdoctoral Science Foundation(2016M590771)Guangdong Natural Science Foundation(2016A030310413,2013B090500027,2014A030310445,2016A050502004)~~
文摘Metal-organic-framework (MOF)-based materials with novel physicochemical properties have emerged as promising catalysts for various hydrogenation reactions. In addition to metal clusters and multifunctional organic ligands, MOF-based catalysts can incorporate other functional species, and thus provide various active sites for hydrogenation processes. The structural properties of the catalysts play significant roles in enhancing the interactions among the reactants, products, and catalytic sites, which can be rationally designed. Because of the synergistic effects between the ac-tive sites and the structural properties, MOF-based catalysts can achieve higher activities and selec- tivities in hydrogenation reactions than can be obtained using traditional heterogeneous catalysts. This review provides an overview of recent developments in MOF-based catalysts in the hydro-genation of alkenes, alkynes, nitroarenes, cinnamaldehyde, furfural, benzene, and other compounds. Strategies for improving the catalytic performances of MOF-based catalysts are discussed as well as the different active sites and structural properties of the catalysts.