The production of renewable fossil fuels such as CH_(4) and CO by photocatalytic CO_(2)reduction has attracted more and more attention.However,single photocatalyst is less efficient for photocatalytic reduction of CO_...The production of renewable fossil fuels such as CH_(4) and CO by photocatalytic CO_(2)reduction has attracted more and more attention.However,single photocatalyst is less efficient for photocatalytic reduction of CO_(2)due to the fast recombination of photogenerated electron pairs.Herein,we successfully prepare CdS-Ag_(2)S composite by assembling the Ag_(2)S QDs cocatalyst on the surface of CdS nanosheet-assembled flower through oil-bath solvothermal method.This composite is prepared through a simple self-assembly strategy using cadmium chloride,ammonia and thiourea as precursors of the CdS nanosheet-assembled flower and silver nitrate and 3-mercaptopropionic acid as the precursors of Ag_(2)S QDs.The average diameter of Ag_(2)S QDs is apparently 6.0 nm.The light absorption edge of the composite is at around 560 nm,with the corresponding band gap at 2.14 eV.The CdS-Ag_(2)S QDs composite with 5 wt%Ag_(2)S QDs loaded achieves CO evolution rate of 16.6μmol·g^(-1)·h^(-1)without noble-metal cocatalysts.This strengthened photocatalytic performance and photocatalytic stability were attributed to the energy band broadening of Ag_(2)S QDs caused by quantum size effect and the large specific surface area due to the assembled flower.The mechanism underlying the enhanced photocatalytic CO_(2)reduction activity is further proposed.This study demonstrates that semiconductor-based quantum dots are strong candidates for excellent cocatalysts in photocatalysis.展开更多
Designing photocatalysts with high light utilization and efficient photogenerated carrier separation for pollutant degradation is one of the important topics for sustainable development.In this study,hierarchical core...Designing photocatalysts with high light utilization and efficient photogenerated carrier separation for pollutant degradation is one of the important topics for sustainable development.In this study,hierarchical core–shell materialα-Fe_(2)O_(3)@ZnIn_(2)S_(4)with a step-scheme(S-scheme)heterojunction is synthesized by in situ growth technique,and MXene Ti_(3)C_(2)quantum dots(QDs)are introduced to construct a double-heterojunction tandem mechanism.The photodegradation efficiency ofα-Fe_(2)O_(3)@ZnIn_(2)S_(4)/Ti_(3)C_(2)QDs to bisphenol A is 96.1%and its reaction rate constant attained 0.02595 min^(−1),which is 12.3 times that of pureα-Fe_(2)O_(3).Meanwhile,a series of characterizations analyze the reasons for the enhanced photocatalytic activity,and the charge transport path of the S-scheme heterojunction/Schottky junction tandem is investigated.The construction of the S-scheme heterojunction enables the photo-generated electrons ofα-Fe_(2)O_(3)and the holes of ZnIn2S4 to transfer and combine under the action of the reverse built-in electric field.Due to the metallic conductivity of Ti_(3)C_(2)QDs,the photogenerated electrons of ZnIn_(2)S_(4)are further transferred to Ti_(3)C_(2)QDs to form a Schottky junction,which in turn forms a double-heterojunction tandem mechanism,showing a remarkable charge separation efficiency.This work provides a new opinion for the construction of tandem double heterojunctions to degrade harmful pollutants.展开更多
基金partially supported by the National Natural Science Foundation of China(No.51672099 and 52073263)the Open Foundation of State Key Laboratory of Electronic Thin Films and Integrated Devices(No.KFJJ202105)Fundamental Research Funds for the Central Universities(No.2017-QR-25)。
文摘The production of renewable fossil fuels such as CH_(4) and CO by photocatalytic CO_(2)reduction has attracted more and more attention.However,single photocatalyst is less efficient for photocatalytic reduction of CO_(2)due to the fast recombination of photogenerated electron pairs.Herein,we successfully prepare CdS-Ag_(2)S composite by assembling the Ag_(2)S QDs cocatalyst on the surface of CdS nanosheet-assembled flower through oil-bath solvothermal method.This composite is prepared through a simple self-assembly strategy using cadmium chloride,ammonia and thiourea as precursors of the CdS nanosheet-assembled flower and silver nitrate and 3-mercaptopropionic acid as the precursors of Ag_(2)S QDs.The average diameter of Ag_(2)S QDs is apparently 6.0 nm.The light absorption edge of the composite is at around 560 nm,with the corresponding band gap at 2.14 eV.The CdS-Ag_(2)S QDs composite with 5 wt%Ag_(2)S QDs loaded achieves CO evolution rate of 16.6μmol·g^(-1)·h^(-1)without noble-metal cocatalysts.This strengthened photocatalytic performance and photocatalytic stability were attributed to the energy band broadening of Ag_(2)S QDs caused by quantum size effect and the large specific surface area due to the assembled flower.The mechanism underlying the enhanced photocatalytic CO_(2)reduction activity is further proposed.This study demonstrates that semiconductor-based quantum dots are strong candidates for excellent cocatalysts in photocatalysis.
基金supported by the National Natural Science Foundation of China(No.21771061)Outstanding Youth Fund of Heilongjiang Province(No.JQ 2020B002).
文摘Designing photocatalysts with high light utilization and efficient photogenerated carrier separation for pollutant degradation is one of the important topics for sustainable development.In this study,hierarchical core–shell materialα-Fe_(2)O_(3)@ZnIn_(2)S_(4)with a step-scheme(S-scheme)heterojunction is synthesized by in situ growth technique,and MXene Ti_(3)C_(2)quantum dots(QDs)are introduced to construct a double-heterojunction tandem mechanism.The photodegradation efficiency ofα-Fe_(2)O_(3)@ZnIn_(2)S_(4)/Ti_(3)C_(2)QDs to bisphenol A is 96.1%and its reaction rate constant attained 0.02595 min^(−1),which is 12.3 times that of pureα-Fe_(2)O_(3).Meanwhile,a series of characterizations analyze the reasons for the enhanced photocatalytic activity,and the charge transport path of the S-scheme heterojunction/Schottky junction tandem is investigated.The construction of the S-scheme heterojunction enables the photo-generated electrons ofα-Fe_(2)O_(3)and the holes of ZnIn2S4 to transfer and combine under the action of the reverse built-in electric field.Due to the metallic conductivity of Ti_(3)C_(2)QDs,the photogenerated electrons of ZnIn_(2)S_(4)are further transferred to Ti_(3)C_(2)QDs to form a Schottky junction,which in turn forms a double-heterojunction tandem mechanism,showing a remarkable charge separation efficiency.This work provides a new opinion for the construction of tandem double heterojunctions to degrade harmful pollutants.