The internal electric field(IEF)is key in speeding up the separation and transfer of photogenerated carriers,which boosts the production of reactive oxygen species(ROS).In this study,we present a novel silver iodide/N...The internal electric field(IEF)is key in speeding up the separation and transfer of photogenerated carriers,which boosts the production of reactive oxygen species(ROS).In this study,we present a novel silver iodide/N-rich carbon nitride(AgI/C_(3)N_(5))heterojunction catalyst with an IEF directed from AgI to C_(3)N_(5).We confirmed this IEF using density functional theory(DFT)calculations and various characterization methods.This IEF induces and reinforces the Type II transfer pathway for carrier separation and transfer,significantly increasing the production of ROS,particularly singlet oxygen(1O_(2)).As a result,the AgI/C_(3)N_(5)catalysts achieve 10.1 times the disinfection efficiency of C_(3)N_(5)and 5.6 times that of AgI,under one-min reaction time,107 CFU/mL of E.coli,visible light,and room temperature.It also outperforms most other AgI and carbon nitride-based heterojunction photocatalysts.Notably,the photogenerated holes(h+)selectively oxidize superoxide radicals(·O_(2)^(-))to 1O_(2)due to favorable energy alignment,minimizing O_(2)reduction effects and enhancing photocorrosion resistance,as demonstrated in five consecutive cycling experiments.In addition,the actual water disinfection tests confirmed its practical application potential.This work highlights the AgI/C_(3)N_(5)heterojunction catalyst’s promise as an efficient disinfection agent and sheds light on the photocatalytic disinfection mechanism.展开更多
A nitrogen-containing ionic liquid was synthesized using an aromatic nitrogen-containing heterocyclic and an amino acid,and applied to the extractive desulfurization process to remove benzothiophene,dibenzothiophene,a...A nitrogen-containing ionic liquid was synthesized using an aromatic nitrogen-containing heterocyclic and an amino acid,and applied to the extractive desulfurization process to remove benzothiophene,dibenzothiophene,and 4,6-dimethyldibenzothiphene from a model fuel oil.Chemical characterizations and simulation using Gaussian 09 software confirmed the rationality of an ionic liquid structure.Classification of non-covalent interactions between the ionic liquid and the three sulfur-containing contaminants was studied by reduced density gradient analysis.The viscosity of the ionic liquid was adjusted by addition of polyethylene glycol.Under extraction conditions of the volume of ionic liquid to oil as 1:1 and temperature as room temperature,the desulfurization selectivity of ionic liquid followed the order of 4,6-dimethyldibenzothiphene(15 min)<benzothiophene(15 min)≈dibenzothiophene(10 min).Addition of p-xylene and cyclohexene to the fuel oil had little effect.The extractant remained stable and effective after multiple regeneration cycles.展开更多
基金supported by National Natural Science Foundation of China(Grant No.52300218 and 22476066)Yunnan Fundamental Research Projects(Grant No.202401CF070197).
文摘The internal electric field(IEF)is key in speeding up the separation and transfer of photogenerated carriers,which boosts the production of reactive oxygen species(ROS).In this study,we present a novel silver iodide/N-rich carbon nitride(AgI/C_(3)N_(5))heterojunction catalyst with an IEF directed from AgI to C_(3)N_(5).We confirmed this IEF using density functional theory(DFT)calculations and various characterization methods.This IEF induces and reinforces the Type II transfer pathway for carrier separation and transfer,significantly increasing the production of ROS,particularly singlet oxygen(1O_(2)).As a result,the AgI/C_(3)N_(5)catalysts achieve 10.1 times the disinfection efficiency of C_(3)N_(5)and 5.6 times that of AgI,under one-min reaction time,107 CFU/mL of E.coli,visible light,and room temperature.It also outperforms most other AgI and carbon nitride-based heterojunction photocatalysts.Notably,the photogenerated holes(h+)selectively oxidize superoxide radicals(·O_(2)^(-))to 1O_(2)due to favorable energy alignment,minimizing O_(2)reduction effects and enhancing photocorrosion resistance,as demonstrated in five consecutive cycling experiments.In addition,the actual water disinfection tests confirmed its practical application potential.This work highlights the AgI/C_(3)N_(5)heterojunction catalyst’s promise as an efficient disinfection agent and sheds light on the photocatalytic disinfection mechanism.
基金This work was supported by the National Natural Science Foundation of China(Grant Nos.22125802,22078010 and U1862113)the Big Science Project from BUCT(Grant No.XK180301).
文摘A nitrogen-containing ionic liquid was synthesized using an aromatic nitrogen-containing heterocyclic and an amino acid,and applied to the extractive desulfurization process to remove benzothiophene,dibenzothiophene,and 4,6-dimethyldibenzothiphene from a model fuel oil.Chemical characterizations and simulation using Gaussian 09 software confirmed the rationality of an ionic liquid structure.Classification of non-covalent interactions between the ionic liquid and the three sulfur-containing contaminants was studied by reduced density gradient analysis.The viscosity of the ionic liquid was adjusted by addition of polyethylene glycol.Under extraction conditions of the volume of ionic liquid to oil as 1:1 and temperature as room temperature,the desulfurization selectivity of ionic liquid followed the order of 4,6-dimethyldibenzothiphene(15 min)<benzothiophene(15 min)≈dibenzothiophene(10 min).Addition of p-xylene and cyclohexene to the fuel oil had little effect.The extractant remained stable and effective after multiple regeneration cycles.
