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
Density functional theory (DFT) simulation was performed to investigate the adsorption mechanisms between frothers and gas–liquid interface. In water phase, the polar head group of the frother molecule was connected ...Density functional theory (DFT) simulation was performed to investigate the adsorption mechanisms between frothers and gas–liquid interface. In water phase, the polar head group of the frother molecule was connected with water molecules by hydrogen bonding, while the non-polar group showed that hydrophobic property and water molecules around it were repelled away. The adsorption of water molecules on single frother molecule suggests that the complexes of α-terpineol-7H2O, MIBC-7H2O and DF200-13H2O reach their stable structure. The hydration shell affects both the polar head group and the non-polar group. The liquid film drainage rate of DF200 is the lowest, while α-terpineol and MIBC are almost the same. The adsorption layer of frother molecules adsorbed at the gas-liquid interface reveals that the α-terpineol molecules are more neatly arranged and better distributed. The DF200 molecules are arranged much more loosely than MIBC molecules. These results suggest that the α-terpineol molecule layer could better block the diffusion of gas through the liquid film than DF200 and MIBC. The simulation results indicate that the foam stability of α-terpineol is the best, followed by DF200 and MIBC.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Projects(51574092,51874106)supported by the National Natural Science Foundation,ChinaProject supported by Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund(the second phase),China
文摘Density functional theory (DFT) simulation was performed to investigate the adsorption mechanisms between frothers and gas–liquid interface. In water phase, the polar head group of the frother molecule was connected with water molecules by hydrogen bonding, while the non-polar group showed that hydrophobic property and water molecules around it were repelled away. The adsorption of water molecules on single frother molecule suggests that the complexes of α-terpineol-7H2O, MIBC-7H2O and DF200-13H2O reach their stable structure. The hydration shell affects both the polar head group and the non-polar group. The liquid film drainage rate of DF200 is the lowest, while α-terpineol and MIBC are almost the same. The adsorption layer of frother molecules adsorbed at the gas-liquid interface reveals that the α-terpineol molecules are more neatly arranged and better distributed. The DF200 molecules are arranged much more loosely than MIBC molecules. These results suggest that the α-terpineol molecule layer could better block the diffusion of gas through the liquid film than DF200 and MIBC. The simulation results indicate that the foam stability of α-terpineol is the best, followed by DF200 and MIBC.
