The design and development of a highly robust catalyst for energy production and environmental abetment are gaining much attention in the field of visible-light-driven catalysis.This work demonstrates the fabrication ...The design and development of a highly robust catalyst for energy production and environmental abetment are gaining much attention in the field of visible-light-driven catalysis.This work demonstrates the fabrication of a series of hierarchical macroporous mixed-phase TiO_(2)on the surface of B-doped g-C_(3)N_(4)(BCN).The physicochemical properties such as crystallinity,morphology,chemical environment,and optical and electronic properties of the as-synthesized materials were analysed by using different analytical techniques.PXRD and HRTEM data revealed the growth of mixed-phase TiO_(2)(anatase and rutile)on the BCN surface,mimicking P25 in the case of the best photocatalyst(TBCN-8).The catalytic activity of the as-synthesized materials was tested towards H2O_(2)production(110μmol h-1)and phenol oxidation(87% of 20 ppm phenol solution)under visible light.Higher photocurrent,lower impedance arc,and lower PL intensity suggest a lower electron-hole recombination rate in the case of TBCN-8,elucidating the best catalytic performance by the material.This work validates the facile fabrication of macroporous TiO_(2)/BCN nanocomposites and their visible-light-driven catalytic activity based on both the p-n heterojunction and Z-scheme mechanism.展开更多
To achieve the United Nations’Sustainable Development Goal(SDG7)of limiting global temperature rise to less than 1.5℃,it is crucial to reduce non-renewable energy sources and curb the production of greenhouse gases ...To achieve the United Nations’Sustainable Development Goal(SDG7)of limiting global temperature rise to less than 1.5℃,it is crucial to reduce non-renewable energy sources and curb the production of greenhouse gases like CO_(2).In this context,graphitic carbon nitride(g-C_(3)N_(4))has emerged as a promising metal-free semiconductor photocatalyst for converting solar energy into clean fuels and valuable chemicals.However,there are challenges associated with g-C_(3)N_(4),such as high electron-hole recombination,low photocurrent generation,limited specific surface area,and an absorption edge below 450 nm,which can be attributed to the arrangement of monomeric units.This review focuses on recent developments in designing single g-C_(3)N_(4) as a metal-free catalyst through atomic-level doping and tuning surface chemical properties.Various doping techniques,including nonmetal and bi-nonmetal doping,as well as vacancy creation within the polymer framework and the effect of surface plasmonic nanoparticles,are explored as effective ways to fine-tune the polymer’s conduction band(CB)edge potential,bandgap,and structural properties.The impact of doping and vacancy creation on the distribution of molecular orbitals,density of states(DOS),and adsorption energy on the polymer surface is investigated using computational calculations based on first principles and density functional theory(DFT).The review also examines the influence of doping on the photocatalytic reactions occurring in the polymer’s CB,such as water splitting and carbon dioxide(CO_(2))reduction,and their selectivity in producing desired products.Last,the review summarizes the current challenges.It provides future perspectives on developing metal-free photocatalysts,emphasizing the need to address unresolved structural,electronic,chemical,and optical properties to advance sustainable solutions.Overall,it is hoped that this review will inspire further research to unlock the full potential of metal-free photocatalysts and contribute to a more sustainable future.展开更多
文摘The design and development of a highly robust catalyst for energy production and environmental abetment are gaining much attention in the field of visible-light-driven catalysis.This work demonstrates the fabrication of a series of hierarchical macroporous mixed-phase TiO_(2)on the surface of B-doped g-C_(3)N_(4)(BCN).The physicochemical properties such as crystallinity,morphology,chemical environment,and optical and electronic properties of the as-synthesized materials were analysed by using different analytical techniques.PXRD and HRTEM data revealed the growth of mixed-phase TiO_(2)(anatase and rutile)on the BCN surface,mimicking P25 in the case of the best photocatalyst(TBCN-8).The catalytic activity of the as-synthesized materials was tested towards H2O_(2)production(110μmol h-1)and phenol oxidation(87% of 20 ppm phenol solution)under visible light.Higher photocurrent,lower impedance arc,and lower PL intensity suggest a lower electron-hole recombination rate in the case of TBCN-8,elucidating the best catalytic performance by the material.This work validates the facile fabrication of macroporous TiO_(2)/BCN nanocomposites and their visible-light-driven catalytic activity based on both the p-n heterojunction and Z-scheme mechanism.
基金supported by Basic Science Research Program through the National Research Foundation of Korean government(MSIT)(2022R1A2C3004242)partly by the Ministry of Trade,Industry Energy(MOTIE)of the Republic of Korea under Grant No.20019175.
文摘To achieve the United Nations’Sustainable Development Goal(SDG7)of limiting global temperature rise to less than 1.5℃,it is crucial to reduce non-renewable energy sources and curb the production of greenhouse gases like CO_(2).In this context,graphitic carbon nitride(g-C_(3)N_(4))has emerged as a promising metal-free semiconductor photocatalyst for converting solar energy into clean fuels and valuable chemicals.However,there are challenges associated with g-C_(3)N_(4),such as high electron-hole recombination,low photocurrent generation,limited specific surface area,and an absorption edge below 450 nm,which can be attributed to the arrangement of monomeric units.This review focuses on recent developments in designing single g-C_(3)N_(4) as a metal-free catalyst through atomic-level doping and tuning surface chemical properties.Various doping techniques,including nonmetal and bi-nonmetal doping,as well as vacancy creation within the polymer framework and the effect of surface plasmonic nanoparticles,are explored as effective ways to fine-tune the polymer’s conduction band(CB)edge potential,bandgap,and structural properties.The impact of doping and vacancy creation on the distribution of molecular orbitals,density of states(DOS),and adsorption energy on the polymer surface is investigated using computational calculations based on first principles and density functional theory(DFT).The review also examines the influence of doping on the photocatalytic reactions occurring in the polymer’s CB,such as water splitting and carbon dioxide(CO_(2))reduction,and their selectivity in producing desired products.Last,the review summarizes the current challenges.It provides future perspectives on developing metal-free photocatalysts,emphasizing the need to address unresolved structural,electronic,chemical,and optical properties to advance sustainable solutions.Overall,it is hoped that this review will inspire further research to unlock the full potential of metal-free photocatalysts and contribute to a more sustainable future.
