Hydrogen production through solar energy is one of the most important pathways to meet the growing demand of renewable energy,and photocatalyst participation in solar hydrolytic hydrogen production has received great ...Hydrogen production through solar energy is one of the most important pathways to meet the growing demand of renewable energy,and photocatalyst participation in solar hydrolytic hydrogen production has received great attention in recent years in terms of low cost,high efficiency,and flexible design.Particularly,g-C_(3)N_(4)(Graphitic-like carbon nitride material),as a unique material,can catalyze the hydrogen production process by completing the separation and transmission of charge.The easily adjustable pore structure/surface area,dimension,band-gap modulation and defect have shown great potential for hydrogen production from water cracking.In this review,the most recent advance of g-C_(3)N_(4) including the doping of metal and non-metal elements,and the formation of semiconductor heterojunction is highlighted.The main modification strategies and approaches for the design of g-C_(3)N_(4) for hydrogen production,as well as the influence of various materials on hydrogen evolution regarding the photocatalysis mechanism and advantages brought by theoretical calculations are specially and briefly illu-strated.Potential design pathways and strategies of g-C_(3)N_(4) are discussed.In addition,current challenges of hydrogen production from g-C_(3)N_(4) water splitting are summarized and can be expected.展开更多
Metal-free catalyst for photocatalytic production of H_(2)O_(2)is highly desirable with the long-term vision of artificial photosynthesis of solar fuel.In particular,the specific chemical bonds for selective H_(2)O_(2...Metal-free catalyst for photocatalytic production of H_(2)O_(2)is highly desirable with the long-term vision of artificial photosynthesis of solar fuel.In particular,the specific chemical bonds for selective H_(2)O_(2)photosynthesis via 2e–oxygen reduction reactions(ORR)remain to be explored for understanding the forming mechanism of active sites.Herein,we report a facile doping method to introduce boron-nitrogen(B–N)bonds into the structure of graphitic carbon nitride(g-C_(3)N_(4))nanosheets(denoted as BCNNS)to provide significant photocatalytic activity,selectivity and stability.The theoretical calculation and experimental results reveal that the electron-deficient B–N units serving as electron acceptors improve photogenerated charge separation and transfer.The units are also proved to be superior active sites for selective O_(2)adsorption and activation,reducing the energy barrier for*OOH formation,and thereby enabling an efficient 2e–ORR pathway to H_(2)O_(2).Consequently,with only bare loss of activity during repeated cycles,the optimal H2O2 production rate by BCNNS photocatalysts reaches 1.16 mmol·L^(–1)·h^(–1)under 365 nm-monochrome light emitting diode(LED365nm)irradiation,increasing nearly 2–5 times as against the state-of-art metal-free photocatalysts.This work gives the first example of applying B–N bonds to enhance the photocatalytic H_(2)O_(2)production as well as unveiling the underlying reaction pathway for efficient solar-energy transformations.展开更多
Herein,we report the fabrication of Fe_(3)O_(4)@TiO_(2) nanosheet/Ag/g-C_(3)N_(4)(Fe_(3)O_(4)@ns-TiO_(2)/Ag/g-C_(3)N_(4))composite photocatalysts with well-designed hierarchical yolk-shell structure.To endow the compo...Herein,we report the fabrication of Fe_(3)O_(4)@TiO_(2) nanosheet/Ag/g-C_(3)N_(4)(Fe_(3)O_(4)@ns-TiO_(2)/Ag/g-C_(3)N_(4))composite photocatalysts with well-designed hierarchical yolk-shell structure.To endow the composites with fascinating features,multiple functional components are perfectly integrated into the definite structure.The photodegradation experiments of organic pollutants revealed a significant enhancement in photocatalytic activity of developed composites as compared to P25,which is mainly due to the synergetic interaction of the tailored three-dimensional(3D)yolk-shell porous nanostructure,extended sunlight response range,and retarded the recombination probability of photogenerated electrons-holes.More importantly,the hybrid samples exhibited superior magnetic properties due to the magnetic component.The excellent magnetic recyclability and reusability of the photocatalysts are verified by the magnetic hysteresis loop and cyclic photocatalytic degradation experiments,which is significant for the green and sustainable applications of photocatalysts.Considering its remarkable photocatalytic performance and expectant magnetic recyclability,the composite photocatalysts are expected to be a promising candidate to dispose of future environmental issues.展开更多
基金This work was supported by Sichuan Science and Technology Program(2021YFS0284,2018SZDZX0026,2021YFS0289)the Opening Project of Key Laboratory of Theoretical Chemistry of Environment(South China Normal University),Ministry of Education(20200103)+1 种基金the Fundamental Research Funds for the Central Universities of Southwest Jiaotong University(210824)the Opening Project of Key Laboratory of Southwest Jiaotong University(ZD2021210001).
文摘Hydrogen production through solar energy is one of the most important pathways to meet the growing demand of renewable energy,and photocatalyst participation in solar hydrolytic hydrogen production has received great attention in recent years in terms of low cost,high efficiency,and flexible design.Particularly,g-C_(3)N_(4)(Graphitic-like carbon nitride material),as a unique material,can catalyze the hydrogen production process by completing the separation and transmission of charge.The easily adjustable pore structure/surface area,dimension,band-gap modulation and defect have shown great potential for hydrogen production from water cracking.In this review,the most recent advance of g-C_(3)N_(4) including the doping of metal and non-metal elements,and the formation of semiconductor heterojunction is highlighted.The main modification strategies and approaches for the design of g-C_(3)N_(4) for hydrogen production,as well as the influence of various materials on hydrogen evolution regarding the photocatalysis mechanism and advantages brought by theoretical calculations are specially and briefly illu-strated.Potential design pathways and strategies of g-C_(3)N_(4) are discussed.In addition,current challenges of hydrogen production from g-C_(3)N_(4) water splitting are summarized and can be expected.
基金supported by the Jiangsu Provincial Double-Innovation Doctor Program(JSSCBS20210996).
文摘Metal-free catalyst for photocatalytic production of H_(2)O_(2)is highly desirable with the long-term vision of artificial photosynthesis of solar fuel.In particular,the specific chemical bonds for selective H_(2)O_(2)photosynthesis via 2e–oxygen reduction reactions(ORR)remain to be explored for understanding the forming mechanism of active sites.Herein,we report a facile doping method to introduce boron-nitrogen(B–N)bonds into the structure of graphitic carbon nitride(g-C_(3)N_(4))nanosheets(denoted as BCNNS)to provide significant photocatalytic activity,selectivity and stability.The theoretical calculation and experimental results reveal that the electron-deficient B–N units serving as electron acceptors improve photogenerated charge separation and transfer.The units are also proved to be superior active sites for selective O_(2)adsorption and activation,reducing the energy barrier for*OOH formation,and thereby enabling an efficient 2e–ORR pathway to H_(2)O_(2).Consequently,with only bare loss of activity during repeated cycles,the optimal H2O2 production rate by BCNNS photocatalysts reaches 1.16 mmol·L^(–1)·h^(–1)under 365 nm-monochrome light emitting diode(LED365nm)irradiation,increasing nearly 2–5 times as against the state-of-art metal-free photocatalysts.This work gives the first example of applying B–N bonds to enhance the photocatalytic H_(2)O_(2)production as well as unveiling the underlying reaction pathway for efficient solar-energy transformations.
基金The authors gratefully acknowledge the financial support from Jiangsu Agriculture Science and Technology Innovation Fund(JASTIF)(No.CX(18)2025)National Natural Science Foundation of China(No.31871881)+2 种基金S&T Support Program of Jiangsu Province(No.BE2017623)the National First-class Discipline Program of Food Science and Technology(No.JUFSTR20180303)the Distinguished Professor Program of Jiangsu Province.
文摘Herein,we report the fabrication of Fe_(3)O_(4)@TiO_(2) nanosheet/Ag/g-C_(3)N_(4)(Fe_(3)O_(4)@ns-TiO_(2)/Ag/g-C_(3)N_(4))composite photocatalysts with well-designed hierarchical yolk-shell structure.To endow the composites with fascinating features,multiple functional components are perfectly integrated into the definite structure.The photodegradation experiments of organic pollutants revealed a significant enhancement in photocatalytic activity of developed composites as compared to P25,which is mainly due to the synergetic interaction of the tailored three-dimensional(3D)yolk-shell porous nanostructure,extended sunlight response range,and retarded the recombination probability of photogenerated electrons-holes.More importantly,the hybrid samples exhibited superior magnetic properties due to the magnetic component.The excellent magnetic recyclability and reusability of the photocatalysts are verified by the magnetic hysteresis loop and cyclic photocatalytic degradation experiments,which is significant for the green and sustainable applications of photocatalysts.Considering its remarkable photocatalytic performance and expectant magnetic recyclability,the composite photocatalysts are expected to be a promising candidate to dispose of future environmental issues.
