Hydrogen peroxide(H_(2)O_(2))is a versatile oxidant with significant applications,particularly in regulating the microenvironment for healthcare purposes.Herein,a rational design of the photoanode is implemented to en...Hydrogen peroxide(H_(2)O_(2))is a versatile oxidant with significant applications,particularly in regulating the microenvironment for healthcare purposes.Herein,a rational design of the photoanode is implemented to enhance H_(2)O_(2) production by oxidizing H_(2)O in a portable photoelectrocatalysis(PEC)device.The obtained solution from this system is demonstrated for effective bactericidal activity against Staphylococcus aureus and Escherichia coli,while maintaining low toxicity toward hippocampal neuronal cells.The photoanode is achieved by Mo-doped BiVO4 films,which are subsequently loaded with cobalt-porphyrin(Co-py)molecules as a co-catalyst.As a result,the optimal performance for H_(2)O_(2) production rate was achieved at 8.4μmol h^(−1) cm^(−2),which is 1.8 times that of the pristine BiVO4 photoanode.Density functional theory(DFT)simulations reveal that the improved performance results from a 1.1 eV reduction in the energy of the rate-determining step of·OH adsorption by the optimal photoanode.This study demonstrates a PEC approach for promoting H_(2)O_(2) production by converting H_(2)O for antibacterial purposes,offering potential applications in conventionally controlling microenvironments for healthcare applications.展开更多
Photocatalytic oxygen reduction provides a sustainable method for on-site hydrogen peroxide(H_(2)O_(2))synthesis.However,most photocatalysts suffer from moderate kinetics due to sluggish electron transfer and ineffici...Photocatalytic oxygen reduction provides a sustainable method for on-site hydrogen peroxide(H_(2)O_(2))synthesis.However,most photocatalysts suffer from moderate kinetics due to sluggish electron transfer and inefficient oxygen adsorption and activation.Herein,sodium(Na)and potassium(K)are co-incorporated into graphitic carbon nitride(g-C_(3)N_(4))via a stepwise co-doping strategy combining sodium chloride-induced and molten salt-assisted polymerization.Experimental results and density functional theory calculations demonstrate that the synergistic interaction between intralayer Na+ions and interlayer K^(+)ions facilitates charge carrier separation and migration both within and between g-C_(3)N_(4)layers.Additionally,multiple heteroatom sites enhance surface charge polarization and introduce cyano groups,which synergistically promote oxygen molecule(O_(2))adsorption and elevate local proton coverage.Simultaneously,the energy barrier for H_(2)O_(2)desorption on the optimal photocatalyst(5Na/3.3K-CN)is lowered,thus improving H_(2)O_(2)production efficiency.Eventually,5Na/3.3K-CN exhibits an impressive H_(2)O_(2)yield of 2541.6μmol·g^(-1)·h^(-1) in an artificial reactor,which is 10.6 times higher than that of pure g-C_(3)N_(4)(240.2μmol·g^(-1)·h^(-1)).Under natural sunlight outdoors,5Na/3.3K-CN still maintains ultrahigh H_(2)O_(2)photosynthesis efficiency,achieving an H_(2)O_(2)photosynthesis rate of 2068.7μmol·g^(-1)·h^(-1).This work introduces a straightforward method to simultaneously optimize charge transfer and O_(2)activation for boosting H_(2)O_(2)photosynthesis,offering valuable insights toward the real-world deployment of g-C_(3)N_(4)-based photocatalysts in environmental protection and energy conversion.展开更多
基金support from the National Key Technologies R&D Program of China(2022YFE0114800)National Natural Science Foundation of China(22075047),and the 111 Project(D16008)。
文摘Hydrogen peroxide(H_(2)O_(2))is a versatile oxidant with significant applications,particularly in regulating the microenvironment for healthcare purposes.Herein,a rational design of the photoanode is implemented to enhance H_(2)O_(2) production by oxidizing H_(2)O in a portable photoelectrocatalysis(PEC)device.The obtained solution from this system is demonstrated for effective bactericidal activity against Staphylococcus aureus and Escherichia coli,while maintaining low toxicity toward hippocampal neuronal cells.The photoanode is achieved by Mo-doped BiVO4 films,which are subsequently loaded with cobalt-porphyrin(Co-py)molecules as a co-catalyst.As a result,the optimal performance for H_(2)O_(2) production rate was achieved at 8.4μmol h^(−1) cm^(−2),which is 1.8 times that of the pristine BiVO4 photoanode.Density functional theory(DFT)simulations reveal that the improved performance results from a 1.1 eV reduction in the energy of the rate-determining step of·OH adsorption by the optimal photoanode.This study demonstrates a PEC approach for promoting H_(2)O_(2) production by converting H_(2)O for antibacterial purposes,offering potential applications in conventionally controlling microenvironments for healthcare applications.
基金supported by the Program for New Century Talents in University(No.NCET-11-0951)from the Ministry of Education of ChinaKey Laboratory Project Fund of CAS(No.2005DP173065-2016-04).
文摘Photocatalytic oxygen reduction provides a sustainable method for on-site hydrogen peroxide(H_(2)O_(2))synthesis.However,most photocatalysts suffer from moderate kinetics due to sluggish electron transfer and inefficient oxygen adsorption and activation.Herein,sodium(Na)and potassium(K)are co-incorporated into graphitic carbon nitride(g-C_(3)N_(4))via a stepwise co-doping strategy combining sodium chloride-induced and molten salt-assisted polymerization.Experimental results and density functional theory calculations demonstrate that the synergistic interaction between intralayer Na+ions and interlayer K^(+)ions facilitates charge carrier separation and migration both within and between g-C_(3)N_(4)layers.Additionally,multiple heteroatom sites enhance surface charge polarization and introduce cyano groups,which synergistically promote oxygen molecule(O_(2))adsorption and elevate local proton coverage.Simultaneously,the energy barrier for H_(2)O_(2)desorption on the optimal photocatalyst(5Na/3.3K-CN)is lowered,thus improving H_(2)O_(2)production efficiency.Eventually,5Na/3.3K-CN exhibits an impressive H_(2)O_(2)yield of 2541.6μmol·g^(-1)·h^(-1) in an artificial reactor,which is 10.6 times higher than that of pure g-C_(3)N_(4)(240.2μmol·g^(-1)·h^(-1)).Under natural sunlight outdoors,5Na/3.3K-CN still maintains ultrahigh H_(2)O_(2)photosynthesis efficiency,achieving an H_(2)O_(2)photosynthesis rate of 2068.7μmol·g^(-1)·h^(-1).This work introduces a straightforward method to simultaneously optimize charge transfer and O_(2)activation for boosting H_(2)O_(2)photosynthesis,offering valuable insights toward the real-world deployment of g-C_(3)N_(4)-based photocatalysts in environmental protection and energy conversion.
