The limited CO_(2)content in aqueous solution and low adsorption amount of CO_(2)on catalyst surface lead to poor photocatalytic CO_(2)reduction activity and selectivity.Herein,the design and fabrication of a novel ph...The limited CO_(2)content in aqueous solution and low adsorption amount of CO_(2)on catalyst surface lead to poor photocatalytic CO_(2)reduction activity and selectivity.Herein,the design and fabrication of a novel photocatalytic architecture is reported,accomplished via chemical vapor deposition of polymeric carbon nitride on carbon paper.The as-obtained samples with a hydrophobic surface exhibit excellent CO_(2)transport and adsorption ability,as well as the building of triphase air-liquid-solid(CO_(2)-H_(2)O-catalyst)joint interfaces,eventually resulting in the inhibition of H2 evolution and great promotion of CO_(2)reduction with a selectivity of 78.6%.The addition of phosphate to reaction environment makes further improvement of CO_(2)photoreduction into carbon fuels with a selectivity of 93.8%and an apparent quantum yield of 0.4%.This work provides new insight for constructing efficient photocatalytic architecture of CO_(2)photoreduction in aqueous solution and demonstrates that phosphate could play a key role in this process.展开更多
abstract The volumetric mass transfer coefficient kLa of gases （H2, CO, CO2） and mass transfer coefficient kL on liquid par-affin side were studied using the dynamic absorption method in slurry bubble column reactor...abstract The volumetric mass transfer coefficient kLa of gases （H2, CO, CO2） and mass transfer coefficient kL on liquid par-affin side were studied using the dynamic absorption method in slurry bubble column reactors under elevated temperature and elevated pressure. Meanwhile, gas-holdup and gas-liquid interfacial area a were obtained. The effects of temperature, pressure, superficial gas velocity and solid concentration on the mass transfer coeffi-cient were discussed. Experimental results show that the gas-liquid volumetric mass transfer coefficient kLa and interfacial area a increased with the increase of pressure, temperature, and superficial gas velocity, and decreased with the slurry concentration. The mass transfer coefficient kL increased with increasing superficial gas velocity and temperature and decreased with higher slurry concentration, while it changed slightly with pressure. Ac-cording to analysis of experimental data, an empirical correlation is obtained to calculate the values of kLa for H2 （CO, CO2） in the gas-paraffin-quartz system in a bubble column under elevated temperature and elevated pressure.展开更多
文摘The limited CO_(2)content in aqueous solution and low adsorption amount of CO_(2)on catalyst surface lead to poor photocatalytic CO_(2)reduction activity and selectivity.Herein,the design and fabrication of a novel photocatalytic architecture is reported,accomplished via chemical vapor deposition of polymeric carbon nitride on carbon paper.The as-obtained samples with a hydrophobic surface exhibit excellent CO_(2)transport and adsorption ability,as well as the building of triphase air-liquid-solid(CO_(2)-H_(2)O-catalyst)joint interfaces,eventually resulting in the inhibition of H2 evolution and great promotion of CO_(2)reduction with a selectivity of 78.6%.The addition of phosphate to reaction environment makes further improvement of CO_(2)photoreduction into carbon fuels with a selectivity of 93.8%and an apparent quantum yield of 0.4%.This work provides new insight for constructing efficient photocatalytic architecture of CO_(2)photoreduction in aqueous solution and demonstrates that phosphate could play a key role in this process.
基金Supported by the National Natural Science Foundation of China(20776018)the Importation and Development of High-Caliber Talents Project of Beijing Municipal Institutions(CIT&TCD20130325)
文摘abstract The volumetric mass transfer coefficient kLa of gases （H2, CO, CO2） and mass transfer coefficient kL on liquid par-affin side were studied using the dynamic absorption method in slurry bubble column reactors under elevated temperature and elevated pressure. Meanwhile, gas-holdup and gas-liquid interfacial area a were obtained. The effects of temperature, pressure, superficial gas velocity and solid concentration on the mass transfer coeffi-cient were discussed. Experimental results show that the gas-liquid volumetric mass transfer coefficient kLa and interfacial area a increased with the increase of pressure, temperature, and superficial gas velocity, and decreased with the slurry concentration. The mass transfer coefficient kL increased with increasing superficial gas velocity and temperature and decreased with higher slurry concentration, while it changed slightly with pressure. Ac-cording to analysis of experimental data, an empirical correlation is obtained to calculate the values of kLa for H2 （CO, CO2） in the gas-paraffin-quartz system in a bubble column under elevated temperature and elevated pressure.
