Glycerol carbonate,an important glycerol value-added product,has been widely used as an active intermediate and inert solvent in the synthesis of cosmetics,detergents,chemical intermediates,polymers,and so on.The dire...Glycerol carbonate,an important glycerol value-added product,has been widely used as an active intermediate and inert solvent in the synthesis of cosmetics,detergents,chemical intermediates,polymers,and so on.The direct carbonylation from glycerol with CO_(2)is considered a promising route,but still tough work due to the thermodynamic stability and the kinetic inertness of CO_(2).In this work,highlyselective direct carbonylation of glycerol and CO_(2)into glycerol carbonate has been achieved over highly dispersed MgInCe-mixed metal oxides(MgInCe-MMO),which were prepared through the topological transformation derived from the MgInCe-layered double hydroxides(MgInCe-LDHs).By precisely modulating the surface basic-acidic properties and the oxygen vacancies,an efficient carbonylation of glycerol with CO_(2)has been achieved with a selectivity of up to>99%to glycerol carbonate.Deep investigation into the synergistic catalysis of base-acid sites and oxygen vacancies has been clarified.展开更多
The development of highly efficient and earth-abundant oxygen evolution/ reduction reaction (OER/ORR) catalysts is essential for rechargeable metal-air batteries. Herein, cobalt-based hydroxide nanoparticles @ N-dop...The development of highly efficient and earth-abundant oxygen evolution/ reduction reaction (OER/ORR) catalysts is essential for rechargeable metal-air batteries. Herein, cobalt-based hydroxide nanoparticles @ N-doping carbonic framework (CoOHCat@NCF) core-shell structures have been designed as highly stable and efficient OER/ORR bifunctional catalysts. The obtained composite shows enhanced catalytic activities and excellent stability in alkaline media. In the OER, a high turnover frequency (2.03 s^-1 at an overpotential of 0.36 V), low overpotential at high current density (100 mA.cm-2 requiring an overpotential of 0.38 V), and excellent stability (100 mA·cm^-2 for one week with no activity loss) have been achieved. Furthermore, although cobalt species-based catalysts are known as good ORR catalysts, their hybridization with NCF obtained from metal organic frameworks successfully enhanced their ORR activities. The efficient activity of CoOHCat@NCF as a bifunctional oxygen electrocatalyst can be ascribed to the core-shell structures stabilizing the active catalytic sites and the porous shell structure favoring electrocatalysis-related mass transport.展开更多
基金Financial support from the National Key Research and Development Program of China(2022YFB3805602)the National Natural Science Foundation of China(22138001,22288102)the Fundamental Research Funds for the Central Universities。
文摘Glycerol carbonate,an important glycerol value-added product,has been widely used as an active intermediate and inert solvent in the synthesis of cosmetics,detergents,chemical intermediates,polymers,and so on.The direct carbonylation from glycerol with CO_(2)is considered a promising route,but still tough work due to the thermodynamic stability and the kinetic inertness of CO_(2).In this work,highlyselective direct carbonylation of glycerol and CO_(2)into glycerol carbonate has been achieved over highly dispersed MgInCe-mixed metal oxides(MgInCe-MMO),which were prepared through the topological transformation derived from the MgInCe-layered double hydroxides(MgInCe-LDHs).By precisely modulating the surface basic-acidic properties and the oxygen vacancies,an efficient carbonylation of glycerol with CO_(2)has been achieved with a selectivity of up to>99%to glycerol carbonate.Deep investigation into the synergistic catalysis of base-acid sites and oxygen vacancies has been clarified.
基金The authors acknowledge financial support from the National Basic Research Program of China (Nos.2013CB932601 and 2014CB239303) and the National Natural Science Foundation of China (No. 21133001).
文摘The development of highly efficient and earth-abundant oxygen evolution/ reduction reaction (OER/ORR) catalysts is essential for rechargeable metal-air batteries. Herein, cobalt-based hydroxide nanoparticles @ N-doping carbonic framework (CoOHCat@NCF) core-shell structures have been designed as highly stable and efficient OER/ORR bifunctional catalysts. The obtained composite shows enhanced catalytic activities and excellent stability in alkaline media. In the OER, a high turnover frequency (2.03 s^-1 at an overpotential of 0.36 V), low overpotential at high current density (100 mA.cm-2 requiring an overpotential of 0.38 V), and excellent stability (100 mA·cm^-2 for one week with no activity loss) have been achieved. Furthermore, although cobalt species-based catalysts are known as good ORR catalysts, their hybridization with NCF obtained from metal organic frameworks successfully enhanced their ORR activities. The efficient activity of CoOHCat@NCF as a bifunctional oxygen electrocatalyst can be ascribed to the core-shell structures stabilizing the active catalytic sites and the porous shell structure favoring electrocatalysis-related mass transport.
基金This work is supported by the National Natural Science Foundation of China (Nos.21133001 and 21303004),and the National Basic Research Program of China (Nos.2013CB932601 and 2014CB239303).