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
Photoelectrochemical(PEC)water splitting is considered as an ideal technology to produce hydrogen.Photogenerated carrier migration is one of the most important roles in the whole process of PEC water splitting.It incl...Photoelectrochemical(PEC)water splitting is considered as an ideal technology to produce hydrogen.Photogenerated carrier migration is one of the most important roles in the whole process of PEC water splitting.It includes bulk transfer inside of the photoelectrode and the exchange at the solid-liquid interface.The energy barriers during the migration process lead to the dramatic recombination of photogenerated hot carrier and the reducing of their redox capacity.Thus,an applied bias voltage should be provided to overcome these energy barriers,which brings the additional loss of energy.Plentiful researches indicate that some methods for the regulation of photogenerated hot carrier,such as p-n junction,unique transfer nanochannel,tandem nanostructure and Z-Scheme transfer structure et al.,show great potential to achieve high-efficient PEC water overall splitting without any applied bias voltage.Up to now,many reviews have summarized and analyzed the methods to enhance the PEC or photocatalysis water splitting from the perspectives of materials,nanostructures and surface modification etc.However,few of them focus on the topic of photogenerated carrier transfer regulation,which is an important and urgent developing technique.For this reason,this review focuses on the regulation of photogenerated carriers generated by the photoelectrodes and summarizes different advanced methods for photogenerated carrier regulation developed in recent years.Some comments and outlooks are also provided at the end of this review.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financially supported by the National Natural Science Foundation of China,China(Grant Nos.41506093)。
文摘Photoelectrochemical(PEC)water splitting is considered as an ideal technology to produce hydrogen.Photogenerated carrier migration is one of the most important roles in the whole process of PEC water splitting.It includes bulk transfer inside of the photoelectrode and the exchange at the solid-liquid interface.The energy barriers during the migration process lead to the dramatic recombination of photogenerated hot carrier and the reducing of their redox capacity.Thus,an applied bias voltage should be provided to overcome these energy barriers,which brings the additional loss of energy.Plentiful researches indicate that some methods for the regulation of photogenerated hot carrier,such as p-n junction,unique transfer nanochannel,tandem nanostructure and Z-Scheme transfer structure et al.,show great potential to achieve high-efficient PEC water overall splitting without any applied bias voltage.Up to now,many reviews have summarized and analyzed the methods to enhance the PEC or photocatalysis water splitting from the perspectives of materials,nanostructures and surface modification etc.However,few of them focus on the topic of photogenerated carrier transfer regulation,which is an important and urgent developing technique.For this reason,this review focuses on the regulation of photogenerated carriers generated by the photoelectrodes and summarizes different advanced methods for photogenerated carrier regulation developed in recent years.Some comments and outlooks are also provided at the end of this review.
