Converting sustainable solar energy into hydrogen energy over semiconductor-based photocatalytic materials provides an alternative to fossil fuel consumption.However,efficient photocatalytic splitting of water to real...Converting sustainable solar energy into hydrogen energy over semiconductor-based photocatalytic materials provides an alternative to fossil fuel consumption.However,efficient photocatalytic splitting of water to realize carbon-free hydrogen production remains a challenge.Heterojunction photocatalysts with well-defined dimensionality and perfectly matched interfaces are promising for achieving highly efficient solar-to-hydrogen conversion.Herein,we report the fabrication of a novel type of protonated graphitic carbon nitride(PCN)/Ti3C2 MXene heterojunctions with strong interfacial interactions.As expected,the two-dimensional(2D)PCN/2D Ti3C2 MXene interface heterojunction achieves a highly improved hydrogen evolution rate(2181μmol∙g‒1)in comparison with bulk g-C3N4(393μmol∙g‒1)and protonated g-C3N4(816μmol∙g‒1).The charge-regulated surfaces of PCN and the accelerated charge transport at the face-to-face 2D/2D Schottky heterojunction interface are the major contributors to the excellent hydrogen evolution performance of the composite photocatalyst.展开更多
Solar-powered photocatalytic hydrogen production from water using semiconductors provides an eco-friendly and promising approach for converting solar energy into hydrogen fuel.Bulk semiconductors generally suffer from...Solar-powered photocatalytic hydrogen production from water using semiconductors provides an eco-friendly and promising approach for converting solar energy into hydrogen fuel.Bulk semiconductors generally suffer from certain limitations,such as poor visible-light utilization,rapid recombination of charge carriers,and low catalytic capability.The key challenge is to develop visible-light-driven heterojunction photocatalysts that are stable and highly active during the water splitting process.Here,we demonstrate the integration of one-dimensional(1D)Cd S nanorods with two-dimensional(2D)1 T-phase dominated WS_(2) nanosheets for constructing mixed-dimensional heterojunctions for the photocatalytic hydrogen evolution reaction(HER).The resulting 1D CdS/2D WS_(2) nanoheterojunction exhibited an ultrahigh hydrogen-evolution activity of~70 mmol·g^(-1)·h^(-1) that was visible to the naked eye,as well as long-term stability under visible light illumination.The results reveal that the synergy of hybrid nanoarchitectures and intimate interfacial contact between the 1D Cd S nanorods and 1T-phase dominated 2D WS_(2) nanosheets facilitates charge carrier transport,which is beneficial for achieving superior hydrogen evolution.展开更多
Rational design and controllable synthesis of visible-light-responsive photocatalysts that exhibit both good hydrogen-producing efficiency and stability in the water splitting reaction are undoubtedly a challenge. Her...Rational design and controllable synthesis of visible-light-responsive photocatalysts that exhibit both good hydrogen-producing efficiency and stability in the water splitting reaction are undoubtedly a challenge. Here we report an integrated CdS nanorod/oxygen-terminated Ti_(3)C_(2)T_(x) MXene nanosheet heterojunction with a high catalytic hydrogen evolution reaction(HER) activity. By incorporating one-dimensional(1D)CdS nanorods onto annealed ultrathin two-dimensional(2D) MXene nanosheets, the mixed-dimensional 1D/2D heterojunction achieved a hydrogen-evolving rate of 8.87 mmol·g^(-1)·h^(-1), much higher than that of bulk CdS and CdS/unmodified MXene hybrid catalysts. The enhanced HER activity and stability of the designed heterojunction catalyst are attributed to the presence of oxygen-containing terminal groups on the surface of thermally treated Ti_(3)C_(2)T_(x) MXene, extended light absorption spectra as well as the precisely constructed intimate Schottky contact, implying an accelerated interfacial charge transfer and efficient, long-term photocatalytic hydrogen production performance. The results demonstrate that oxygen-terminated 2D MXene can be well utilized as a functional platform for the development of novel heterojunction photocatalysts.展开更多
文摘Converting sustainable solar energy into hydrogen energy over semiconductor-based photocatalytic materials provides an alternative to fossil fuel consumption.However,efficient photocatalytic splitting of water to realize carbon-free hydrogen production remains a challenge.Heterojunction photocatalysts with well-defined dimensionality and perfectly matched interfaces are promising for achieving highly efficient solar-to-hydrogen conversion.Herein,we report the fabrication of a novel type of protonated graphitic carbon nitride(PCN)/Ti3C2 MXene heterojunctions with strong interfacial interactions.As expected,the two-dimensional(2D)PCN/2D Ti3C2 MXene interface heterojunction achieves a highly improved hydrogen evolution rate(2181μmol∙g‒1)in comparison with bulk g-C3N4(393μmol∙g‒1)and protonated g-C3N4(816μmol∙g‒1).The charge-regulated surfaces of PCN and the accelerated charge transport at the face-to-face 2D/2D Schottky heterojunction interface are the major contributors to the excellent hydrogen evolution performance of the composite photocatalyst.
文摘Solar-powered photocatalytic hydrogen production from water using semiconductors provides an eco-friendly and promising approach for converting solar energy into hydrogen fuel.Bulk semiconductors generally suffer from certain limitations,such as poor visible-light utilization,rapid recombination of charge carriers,and low catalytic capability.The key challenge is to develop visible-light-driven heterojunction photocatalysts that are stable and highly active during the water splitting process.Here,we demonstrate the integration of one-dimensional(1D)Cd S nanorods with two-dimensional(2D)1 T-phase dominated WS_(2) nanosheets for constructing mixed-dimensional heterojunctions for the photocatalytic hydrogen evolution reaction(HER).The resulting 1D CdS/2D WS_(2) nanoheterojunction exhibited an ultrahigh hydrogen-evolution activity of~70 mmol·g^(-1)·h^(-1) that was visible to the naked eye,as well as long-term stability under visible light illumination.The results reveal that the synergy of hybrid nanoarchitectures and intimate interfacial contact between the 1D Cd S nanorods and 1T-phase dominated 2D WS_(2) nanosheets facilitates charge carrier transport,which is beneficial for achieving superior hydrogen evolution.
基金financially supported by the National Natural Science Foundation of China(22005149,21975129,and 22172077)the Natural Science Foundation of Jiangsu Province(BK20200777 and BK20211573)+1 种基金the Natural Science Foundation of the Higher Education Institutions of Jiangsu Province,China(20KJB430034)the Science Fund for Distinguished Young Scholars,Nanjing Forestry University(JC2019002)。
基金supported by the National Natural Science Foundation of China (22005149, 21975129)Natural Science Foundation of Jiangsu Province (BK20200777)+2 种基金Natural Science Foundation of the Higher Education Institutions of Jiangsu Province, China (20KJB430034)Science Fund for Distinguished Young Scholars, Nanjing Forestry University (JC2019002)Advanced Analysis and Testing Center, Nanjing Forestry University。
文摘Rational design and controllable synthesis of visible-light-responsive photocatalysts that exhibit both good hydrogen-producing efficiency and stability in the water splitting reaction are undoubtedly a challenge. Here we report an integrated CdS nanorod/oxygen-terminated Ti_(3)C_(2)T_(x) MXene nanosheet heterojunction with a high catalytic hydrogen evolution reaction(HER) activity. By incorporating one-dimensional(1D)CdS nanorods onto annealed ultrathin two-dimensional(2D) MXene nanosheets, the mixed-dimensional 1D/2D heterojunction achieved a hydrogen-evolving rate of 8.87 mmol·g^(-1)·h^(-1), much higher than that of bulk CdS and CdS/unmodified MXene hybrid catalysts. The enhanced HER activity and stability of the designed heterojunction catalyst are attributed to the presence of oxygen-containing terminal groups on the surface of thermally treated Ti_(3)C_(2)T_(x) MXene, extended light absorption spectra as well as the precisely constructed intimate Schottky contact, implying an accelerated interfacial charge transfer and efficient, long-term photocatalytic hydrogen production performance. The results demonstrate that oxygen-terminated 2D MXene can be well utilized as a functional platform for the development of novel heterojunction photocatalysts.
