As a new organic conjugated semiconductor,graphitic carbon nitride(g-C_(3)N_(4))is emerging as a fascinating material for various photocatalytic applications due to its adjustable electronic structure,outstanding ther...As a new organic conjugated semiconductor,graphitic carbon nitride(g-C_(3)N_(4))is emerging as a fascinating material for various photocatalytic applications due to its adjustable electronic structure,outstanding thermal endurance,appealing chemical stability,low cost,and environmental friendliness.Nevertheless,unmodified bulk g-C_(3)N_(4) possesses some intrinsic limitations related to poor crystallinity,marginal visible-light harvesting,easy recombination of charge pairs,small surface area,and slow charge migration,which give rise to the low quantum efficiency of photocatalytic reactions.One efficient strategy to overcome these shortcomings is the manipulation of the microstructures of g-C_(3)N_(4).Other than the traditional structure control,mimicking the structures of creatures in nature to design and construct bio-inspired structures is a promising approach to improve the photocatalytic performance of g-C_(3)N_(4) and even g-C_(3)N_(4)-based systems.This review summarizes the recent advances of the traditional structure-control of g-C_(3)N_(4)-based systems,and bio-inspired synthesis of g-C_(3)N_(4)-based systems from two aspects of structural bionics and functional bionics.Furthermore,the fundamentals of bio-inspired design and fabrication of g-C_(3)N_(4)-based systems are introduced in detail.Additionally,the different theoretical calculations,diverse photocatalytic applications and various modification strategies of bio-inspired structured g-C_(3)N_(4)-based systems are recapped.We believe that this work will be a guiding star for future research in the new field of biomimetic photocatalysis.展开更多
It is a great challenge to prepare non-noble metal electrocatalysts toward hydrogen evolution reaction(HER)with large current density.Synergistic electronic and morphological structures of the catalyst have been consi...It is a great challenge to prepare non-noble metal electrocatalysts toward hydrogen evolution reaction(HER)with large current density.Synergistic electronic and morphological structures of the catalyst have been considered as an effective method to improve the catalytic performance,due to the enhanced intrinsic activity and enlarged accessible active sites.Herein,we present novel ternary Co_(1-x)V_(x)P nanoneedle arrays with modulated electronic and morphological structures as an electrocatalyst for highly efficient HER in alkaline solution.The NF@Co1-xVxP catalyst shows a remarkable catalytic ability with low overpotentials of 46 and 226 mV at current densities of 10 and 400 mA cm^(-2),respectively,as well as a small Tafel slope and superior stability.Combining the experimental and computational study,the excellent catalytic performance was attributed to the improved physical and chemical properties(conductivity and surface activity),large active surface area,and fast reaction kinetics.Furthermore,the assembled Co–V based electrolyzer(NF@Co_(1-x)V_(x)–HNNs(+)||NF@Co_(1-x)V_(x)P(-))delivers small full-cell voltages of 1.58,1.75,and 1.92 V at 10,100,and 300 mA cm^(-2),respectively.Our findings provide a systematic understanding on the V–incorporation strategy to promote highly efficient ternary electrocatalysts via synergistic control of morphology and electronic structures.展开更多
文摘As a new organic conjugated semiconductor,graphitic carbon nitride(g-C_(3)N_(4))is emerging as a fascinating material for various photocatalytic applications due to its adjustable electronic structure,outstanding thermal endurance,appealing chemical stability,low cost,and environmental friendliness.Nevertheless,unmodified bulk g-C_(3)N_(4) possesses some intrinsic limitations related to poor crystallinity,marginal visible-light harvesting,easy recombination of charge pairs,small surface area,and slow charge migration,which give rise to the low quantum efficiency of photocatalytic reactions.One efficient strategy to overcome these shortcomings is the manipulation of the microstructures of g-C_(3)N_(4).Other than the traditional structure control,mimicking the structures of creatures in nature to design and construct bio-inspired structures is a promising approach to improve the photocatalytic performance of g-C_(3)N_(4) and even g-C_(3)N_(4)-based systems.This review summarizes the recent advances of the traditional structure-control of g-C_(3)N_(4)-based systems,and bio-inspired synthesis of g-C_(3)N_(4)-based systems from two aspects of structural bionics and functional bionics.Furthermore,the fundamentals of bio-inspired design and fabrication of g-C_(3)N_(4)-based systems are introduced in detail.Additionally,the different theoretical calculations,diverse photocatalytic applications and various modification strategies of bio-inspired structured g-C_(3)N_(4)-based systems are recapped.We believe that this work will be a guiding star for future research in the new field of biomimetic photocatalysis.
基金the National Natural Science Foundation of China(21671096,21603094 and21905180)the Natural Science Foundation of Guangdong Province(2018B030322001 and 2018A030310225)+4 种基金Shenzhen Peacock Plan(KQTD2016022620054656)Shenzhen Key Laboratory Project(ZDSYS201603311013489)the Basic Research Project of the Science and Technology Innovation Commission of Shenzhen(JCYJ20190809115413414)the Science and Technology Development Fund from Macao SAR(FDCT–0102/2019/A2,FDCT–0035/2019/AGJ and FDCT–0154/2019/A3)the Multi-Year Research Grants(MYRG2017–00027–FST and MYRG2018–00003–IAPME)from the University of Macao。
文摘It is a great challenge to prepare non-noble metal electrocatalysts toward hydrogen evolution reaction(HER)with large current density.Synergistic electronic and morphological structures of the catalyst have been considered as an effective method to improve the catalytic performance,due to the enhanced intrinsic activity and enlarged accessible active sites.Herein,we present novel ternary Co_(1-x)V_(x)P nanoneedle arrays with modulated electronic and morphological structures as an electrocatalyst for highly efficient HER in alkaline solution.The NF@Co1-xVxP catalyst shows a remarkable catalytic ability with low overpotentials of 46 and 226 mV at current densities of 10 and 400 mA cm^(-2),respectively,as well as a small Tafel slope and superior stability.Combining the experimental and computational study,the excellent catalytic performance was attributed to the improved physical and chemical properties(conductivity and surface activity),large active surface area,and fast reaction kinetics.Furthermore,the assembled Co–V based electrolyzer(NF@Co_(1-x)V_(x)–HNNs(+)||NF@Co_(1-x)V_(x)P(-))delivers small full-cell voltages of 1.58,1.75,and 1.92 V at 10,100,and 300 mA cm^(-2),respectively.Our findings provide a systematic understanding on the V–incorporation strategy to promote highly efficient ternary electrocatalysts via synergistic control of morphology and electronic structures.