Hydrogen peroxide(H_(2)O_(2))has gained widespread attention as a versatile oxidant and a mild disin-fectant.Here,an electrostatic self-assembly method is applied to couple ZnSe quantum dots(QDs)with a flower-like cov...Hydrogen peroxide(H_(2)O_(2))has gained widespread attention as a versatile oxidant and a mild disin-fectant.Here,an electrostatic self-assembly method is applied to couple ZnSe quantum dots(QDs)with a flower-like covalent organic framework(COF)to form a step-scheme(S-scheme)photocata-lyst for H_(2)O_(2)production.The as-prepared S-scheme photocatalyst exhibits a broad light absorption range with an edge at 810 nm owing to the synergistic effect between the ZnSe QDs and COF.The S-scheme charge-carrier transfer mechanism is validated by performing Fermi level calculations and in-situ X-ray photoelectron and femtosecond transient absorption spectroscopies.Photolumi-nescence,time-resolved photoluminescence,photocurrent response,electrochemical impedance spectroscopy,and electron paramagnetic resonance results show that the S-scheme heterojunction not only promotes charge carrier separation but also boosts the redox ability,resulting in enhanced photocatalytic performance.Remarkably,a 10%-ZnSe QD/COF has excellent photocatalytic H_(2)O_(2)-production activity,and the optimal S-scheme composite with ethanol as the hole scavenger yields a H_(2)O_(2)-production rate of 1895 mol g^(-1)h-1.This study presents an example of a high-performance organic/inorganic S-scheme photocatalyst for H_(2)O_(2)production.展开更多
First-principles calculations show that the pulse laser induced graphite-to-diamond phase transition is related to the lattice stress generated by the excited carriers,termed as "quantum electronic stress(QES)&qu...First-principles calculations show that the pulse laser induced graphite-to-diamond phase transition is related to the lattice stress generated by the excited carriers,termed as "quantum electronic stress(QES)".We found that the excited carriers in graphite generate a large anisotropic QES that increases linearly with the increasing carrier density.Using the QES as a guiding parameter,structural relaxation spontaneously transforms the graphite phase into the diamond phase,as the QES is reduced and minimized.Our results suggest that the concept of QES can be generally applied as a good measure to characterize the pulse laser induced phase transitions,in analogy to pressure induced phase transitions.展开更多
We report on electrical and optical properties of p＋-i-n＋ photodetectors/solar cells based on square millimeter arrays of InP nanowires （NWs） grown on InP substrates. The study includes a sample series where the p...We report on electrical and optical properties of p＋-i-n＋ photodetectors/solar cells based on square millimeter arrays of InP nanowires （NWs） grown on InP substrates. The study includes a sample series where the p＋-segment length was varied between 0 and 250 nm, as well as solar cells with 9.3% efficiency with similar design. The electrical data for all devices display clear rectifying behavior with an ideality factor between 1.8 and 2.5 at 300 K. From spectrally resolved photocurrent measurements, we conclude that the photocurrent generation process depends strongly on the p^-segment length. Without a p＋-segment, photogenerated carriers funneled from the substrate into the NWs contribute strongly to the photocurrent. Adding a p＋-segment decouples the substrate and shifts the depletion region, and collection of photogenerated carriers, to the NWs, in agreement with theoretical modeling. In optimized solar cells, clear spectral signatures of interband transitions in the zinc blende and wurtzite InP layers of the mixed-phase i-segments are observed. Complementary electroluminescence, transmission electron microscopy （TEM）, as well as measurements of the dependence of the photocurrent on angle of incidence and polarization, support our interpretations.展开更多
文摘Hydrogen peroxide(H_(2)O_(2))has gained widespread attention as a versatile oxidant and a mild disin-fectant.Here,an electrostatic self-assembly method is applied to couple ZnSe quantum dots(QDs)with a flower-like covalent organic framework(COF)to form a step-scheme(S-scheme)photocata-lyst for H_(2)O_(2)production.The as-prepared S-scheme photocatalyst exhibits a broad light absorption range with an edge at 810 nm owing to the synergistic effect between the ZnSe QDs and COF.The S-scheme charge-carrier transfer mechanism is validated by performing Fermi level calculations and in-situ X-ray photoelectron and femtosecond transient absorption spectroscopies.Photolumi-nescence,time-resolved photoluminescence,photocurrent response,electrochemical impedance spectroscopy,and electron paramagnetic resonance results show that the S-scheme heterojunction not only promotes charge carrier separation but also boosts the redox ability,resulting in enhanced photocatalytic performance.Remarkably,a 10%-ZnSe QD/COF has excellent photocatalytic H_(2)O_(2)-production activity,and the optimal S-scheme composite with ethanol as the hole scavenger yields a H_(2)O_(2)-production rate of 1895 mol g^(-1)h-1.This study presents an example of a high-performance organic/inorganic S-scheme photocatalyst for H_(2)O_(2)production.
基金supported by the National Natural Science Foundation of China(Grant No.21603210)Chinese Youth 1000 Talents Program+1 种基金the Fundamental Research Funds for the Central Universitiesthe United States Department of Energy Basic Energy Sciences(Grant No.DE-FG0204ER46148)
文摘First-principles calculations show that the pulse laser induced graphite-to-diamond phase transition is related to the lattice stress generated by the excited carriers,termed as "quantum electronic stress(QES)".We found that the excited carriers in graphite generate a large anisotropic QES that increases linearly with the increasing carrier density.Using the QES as a guiding parameter,structural relaxation spontaneously transforms the graphite phase into the diamond phase,as the QES is reduced and minimized.Our results suggest that the concept of QES can be generally applied as a good measure to characterize the pulse laser induced phase transitions,in analogy to pressure induced phase transitions.
文摘We report on electrical and optical properties of p＋-i-n＋ photodetectors/solar cells based on square millimeter arrays of InP nanowires （NWs） grown on InP substrates. The study includes a sample series where the p＋-segment length was varied between 0 and 250 nm, as well as solar cells with 9.3% efficiency with similar design. The electrical data for all devices display clear rectifying behavior with an ideality factor between 1.8 and 2.5 at 300 K. From spectrally resolved photocurrent measurements, we conclude that the photocurrent generation process depends strongly on the p^-segment length. Without a p＋-segment, photogenerated carriers funneled from the substrate into the NWs contribute strongly to the photocurrent. Adding a p＋-segment decouples the substrate and shifts the depletion region, and collection of photogenerated carriers, to the NWs, in agreement with theoretical modeling. In optimized solar cells, clear spectral signatures of interband transitions in the zinc blende and wurtzite InP layers of the mixed-phase i-segments are observed. Complementary electroluminescence, transmission electron microscopy （TEM）, as well as measurements of the dependence of the photocurrent on angle of incidence and polarization, support our interpretations.
