Hydrogen peroxide(H_(2)O_(2))is a versatile oxidant with significant applications,particularly in regulating the microenvironment for healthcare purposes.Herein,a rational design of the photoanode is implemented to en...Hydrogen peroxide(H_(2)O_(2))is a versatile oxidant with significant applications,particularly in regulating the microenvironment for healthcare purposes.Herein,a rational design of the photoanode is implemented to enhance H_(2)O_(2) production by oxidizing H_(2)O in a portable photoelectrocatalysis(PEC)device.The obtained solution from this system is demonstrated for effective bactericidal activity against Staphylococcus aureus and Escherichia coli,while maintaining low toxicity toward hippocampal neuronal cells.The photoanode is achieved by Mo-doped BiVO4 films,which are subsequently loaded with cobalt-porphyrin(Co-py)molecules as a co-catalyst.As a result,the optimal performance for H_(2)O_(2) production rate was achieved at 8.4μmol h^(−1) cm^(−2),which is 1.8 times that of the pristine BiVO4 photoanode.Density functional theory(DFT)simulations reveal that the improved performance results from a 1.1 eV reduction in the energy of the rate-determining step of·OH adsorption by the optimal photoanode.This study demonstrates a PEC approach for promoting H_(2)O_(2) production by converting H_(2)O for antibacterial purposes,offering potential applications in conventionally controlling microenvironments for healthcare applications.展开更多
This study developed a novel heterogeneous Vis-Photo+Fenton-like system by integrating visible-light-responsive Co_(3)O_(4)/TiO_(2) photocatalysis with peroxymonosulfate(PMS)activation for efficient atrazine(ATZ)degra...This study developed a novel heterogeneous Vis-Photo+Fenton-like system by integrating visible-light-responsive Co_(3)O_(4)/TiO_(2) photocatalysis with peroxymonosulfate(PMS)activation for efficient atrazine(ATZ)degradation.The synergistic process achieved complete ATZ removal within 60 min under near-neutral pH(6.9),outperform-ing individual Fenton-like(39%)and photocatalytic(24%)processes.Key factors influencing the degradation efficiency included light sources(UV>visible),pH(optimal at 6.9),catalyst dosage(0.01 g Co_(3)O_(4)/TiO_(2)),and PMS:ATZ molar ratio(1:2).The system exhibited a synergistic coefficient of 5.03(degradation)and 1.97(miner-alization),attributed to enhanced radical generation and accelerated Co^(3+)/Co^(2+)redox cycling through photoin-duced electron transfer.Intermediate analysis revealed dealkylation,dechlorination,and oxidation pathways,with reduced toxicity of by-products(e.g.,CEAT,CIAT)confirmed by ecotoxicity assessments.The mineralization efficiency(Vis-Photo+Fenton-like)reached 83.1%,significantly higher than that of standalone processes(Fenton-like:43.2%;photocatalysis:30.5%).The catalyst demonstrated excellent stability(nearly 90%recov-ery,<1μg/L Co leaching)and practical applicability.This study provides an efficient,sludge-free,and solar-compatible strategy for eliminating persistent herbicides in water treatment.展开更多
Photocatalytic carbon dioxide(CO_(2))reduction offers an alternative strategy for converting CO_(2)into high-value added gaseous fuels,thereby paving the way for the development of clean and renewable energy.Metal-org...Photocatalytic carbon dioxide(CO_(2))reduction offers an alternative strategy for converting CO_(2)into high-value added gaseous fuels,thereby paving the way for the development of clean and renewable energy.Metal-organic frameworks(MOFs),characterized by their highly porous structure,exceptional CO_(2)adsorption capacity,and tunable architecture,have emerged as promising candidates for photocatalytic CO_(2)reduction.This review systematically examines the recent advancement in MOFs-based photocatalysts for CO_(2)reduction to CO.It begins with the overview of the fundamental mechanisms and processes of MOFs towards photocatalytic CO_(2)reduction.Subsequently,common strategies for the modulation of MOFs-based photocatalysts are summarized,including metallic site modification,functionalized ligand incorporation,morphological control,defect engineering,and heterostructure construction.Notably,the review analyzes the critical factors contributing to the high selectivity of CO_(2)photoreduction to CO from both thermodynamic and kinetic perspectives.The conclusion addresses current challenges and future perspectives in designing highly efficient photocatalysts with abundant active sites,providing valuable insights for their continued development.展开更多
Photocatalytic oxygen reduction provides a sustainable method for on-site hydrogen peroxide(H_(2)O_(2))synthesis.However,most photocatalysts suffer from moderate kinetics due to sluggish electron transfer and ineffici...Photocatalytic oxygen reduction provides a sustainable method for on-site hydrogen peroxide(H_(2)O_(2))synthesis.However,most photocatalysts suffer from moderate kinetics due to sluggish electron transfer and inefficient oxygen adsorption and activation.Herein,sodium(Na)and potassium(K)are co-incorporated into graphitic carbon nitride(g-C_(3)N_(4))via a stepwise co-doping strategy combining sodium chloride-induced and molten salt-assisted polymerization.Experimental results and density functional theory calculations demonstrate that the synergistic interaction between intralayer Na+ions and interlayer K^(+)ions facilitates charge carrier separation and migration both within and between g-C_(3)N_(4)layers.Additionally,multiple heteroatom sites enhance surface charge polarization and introduce cyano groups,which synergistically promote oxygen molecule(O_(2))adsorption and elevate local proton coverage.Simultaneously,the energy barrier for H_(2)O_(2)desorption on the optimal photocatalyst(5Na/3.3K-CN)is lowered,thus improving H_(2)O_(2)production efficiency.Eventually,5Na/3.3K-CN exhibits an impressive H_(2)O_(2)yield of 2541.6μmol·g^(-1)·h^(-1) in an artificial reactor,which is 10.6 times higher than that of pure g-C_(3)N_(4)(240.2μmol·g^(-1)·h^(-1)).Under natural sunlight outdoors,5Na/3.3K-CN still maintains ultrahigh H_(2)O_(2)photosynthesis efficiency,achieving an H_(2)O_(2)photosynthesis rate of 2068.7μmol·g^(-1)·h^(-1).This work introduces a straightforward method to simultaneously optimize charge transfer and O_(2)activation for boosting H_(2)O_(2)photosynthesis,offering valuable insights toward the real-world deployment of g-C_(3)N_(4)-based photocatalysts in environmental protection and energy conversion.展开更多
Photosynthesis is a promising method for H_(2)O_(2)production,but its application in pure water is limited by slow oxidation kinetics and rapid photocarrier recombination of photocatalysts.Herein,a novel defective car...Photosynthesis is a promising method for H_(2)O_(2)production,but its application in pure water is limited by slow oxidation kinetics and rapid photocarrier recombination of photocatalysts.Herein,a novel defective carbon nitride photocatalyst(D-C3-xN4)containing the C vacancies and the frustrated Lewis pairs(B and N of cyano group)is designed for H_(2)O_(2)photosynthesis,and the role of C vacancies on the electron transfer mechanism during photocatalysis is systematically investigated.The D-C_(3-x)N_(4) exhibits a H_(2)O_(2)production rate of 140.1μmol·g^(-1)·h^(-1) in pure water,which is 87.6 times that of C_(3)N_(4).Such superior performance for H_(2)O_(2)photosynthesis is found to arise from the C vacancies and frustrated Lewis pairs(FLPs).The C vacancies have strong electron-trapping ability,which greatly enhances the separation of photocarriers.The C vacancies can also effectively reduce O_(2)to*OOH via a proton-coupled process,which significantly accelerates the O_(2)reduction kinetics.Meanwhile,the FLPs show an outstanding catalytic activity for H_(2)O oxidation.This study not only provides a new structure for highly active photocatalysts,but also deepens the understanding of the electron transfer mechanism of photocatalysts with trapped sites.展开更多
Single-atom catalysts based on graphitic carbon nitride(g-C_(3)N_(4))show high potential for hydrogen production photocatalytically.However,it is still a challenge to develop single-atom-based g-C_(3)N_(4)due to the c...Single-atom catalysts based on graphitic carbon nitride(g-C_(3)N_(4))show high potential for hydrogen production photocatalytically.However,it is still a challenge to develop single-atom-based g-C_(3)N_(4)due to the complex synthesis procedures,limited active sites,and insufficient mechanistic understanding.Herein,a facile oxygen-tolerant synthesis strategy was developed,which utilizes the nitrogen-rich structure of g-C_(3)N_(4)to capture Fe single atoms from ammonium iron citrate,successfully constructing an efficient photocatalytic composite.The resulting Fe single-atom-modified g-C_(3)N_(4)catalyst exhibited highly improved light absorption,charge carrier separation,and a substantially enhanced rate of H_(2)production photocatalytically under visible light irradiation.Experimental results demonstrated that the optimal sample achieves a H_(2)production rate of 683μmol·h-1·g^(-1),representing a 425% enhancement compared to pristine g-C_(3)N_(4).This study presents a facile oxygen-tolerant approach for metal immobilization using metal-organic precursors,where the nitrogen-rich framework of g-C_(3)N_(4)effectively captures Fe atoms as singular site within the composite.The developed synthesis strategy provides new insights for designing high-performance single-atom photocatalytic materials,potentially advancing the application and development of photocatalysis.展开更多
Drug-resistant bacteria,using their dense cell membranes as strong barrier,significantly reduce the efficacy of conventional antibacterial treatments.Phototriggered 2D catalytic nanomaterials have emerged as promising...Drug-resistant bacteria,using their dense cell membranes as strong barrier,significantly reduce the efficacy of conventional antibacterial treatments.Phototriggered 2D catalytic nanomaterials have emerged as promising candidates against drug-resistant bacteria by inducing membrane mechanical damage and generating reactive oxygen species(ROS).However,the practical antibacterial efficacy of typical 2D graphitic carbon nitride(g-C_(3)N_(4))is severely limited due to the low ROS production.Herein,we report an interfacial band-engineered lamellar heterojunctions(MnCN LHJs)through in situ Mn_(2)O_(3)growth on g-C_(3)N_(4).The charges generated in g-C_(3)N_(4)are stabilized by Mn_(2)O_(3),minimizing electron-hole recombination and boosting ROS production.Meanwhile,the photocatalytic effect of MnCN LHJs works synergistically with photothermal effects of Mn_(2)O_(3)to induce a robust“melee attack”against drug-resistant bacteria.High-resolution synchrotron radiation X-ray tomography directly visualized that MnCN LHJs possessed bacterial trapping capabilities,revealing their ability to induce mechanical damage to bacteria membrane for the first time.Additionally,MnCN LHJs can deplete endogenous glutathione,thereby enhancing ROS generation and weakening the bacterial antioxidant defense system.These combined effects achieve a remarkable bactericidal rate exceeding 98% against methicillin-resistant Staphylococcus aureus(MRSA).Notably,MnCN LHJs demonstrate prolonged retention at wound sites,helping to reduce inflammation and promote angiogenesis in infected wounds.This work not only advances interfacial band engineering approach to enhance the photocatalytic performance of g-C_(3)N_(4)but also underscores the significance of nanomaterial-bacteria interaction in design of next-generation antibacterial materials.展开更多
The integration of carbon dots(CDs)with graphitic carbon nitride(g-C_(3)N_(4))has emerged as a promising approach to enhance photocatalytic hydrogen(H_(2))evolution.Despite significant progress,critical challenges rem...The integration of carbon dots(CDs)with graphitic carbon nitride(g-C_(3)N_(4))has emerged as a promising approach to enhance photocatalytic hydrogen(H_(2))evolution.Despite significant progress,critical challenges remain in achieving broad visiblelight absorption and suppressing charge recombination.In this work,we developed a series of photocatalysts through in situ embedding of red-emissive CDs(R-CDs)into g-C_(3)N_(4)(RCN)with precisely controlled loading amounts.Systematic characterization revealed that the R-CDs incorporation simultaneously addresses two fundamental limitations:(1)extending the light absorption edge to 800 nm,and(2)acting as an electron acceptor,facilitating charge separation.The optimized RCN composite demonstrates exceptional H_(2)evolution activity(1.87 mmol·g^(-1)·h^(-1),wavelength(λ)≥420 nm),representing a 3.3-fold enhancement over pristine g-C_(3)N_(4).Remarkably,the apparent quantum efficiency(AQE)reaches 9.1% at 420 nm,while maintaining measurable activity beyond 475 nm,where unmodified g-C_(3)N_(4)shows negligible response.This study provides fundamental insights into band structure engineering and charge carrier management through rational design of CDs-modified semiconductor heterostructures.展开更多
Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-...Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-C_(3)N_(4) suffers from limited visible-light absorption and low charge-carrier mobility.In this study,a phosphorus-doped tubular carbon nitride(5P-TCN)was synthesized via a precursor self-assembly method using phosphoric acid and melamine as raw materials,eliminating the need for organic solvents or templates.The 5P-TCN catalyst demonstrated enhanced visible-light absorption,improved charge transfer capability,and a 5.25-fold increase in specific surface area(31.092 m^(2)/g),which provided abundant active sites to efficiently drive the PMS-assisted photocatalytic reaction.The 5P-TCN/vis/PMS system exhibited exceptional degradation performance for organic pollutants across a broad pH range(3–9),achieving over 92%degradation of Rhodamine B(RhB)within 15 min.Notably,the system retained>98%RhB degradation efficiency after three consecutive operational cycles,demonstrating robust operational stability and reusability.Moreover,key parameters influencing,active radi-cals,degradation pathways,and potential mechanisms for RhB degradation were systematically investigated.This work proposes a green and cost-effective strategy for developing high-efficiency photocatalysts,while demon-strating the exceptional capability of a PMS-assisted photocatalytic system for rapid degradation of RhB.展开更多
基金support from the National Key Technologies R&D Program of China(2022YFE0114800)National Natural Science Foundation of China(22075047),and the 111 Project(D16008)。
文摘Hydrogen peroxide(H_(2)O_(2))is a versatile oxidant with significant applications,particularly in regulating the microenvironment for healthcare purposes.Herein,a rational design of the photoanode is implemented to enhance H_(2)O_(2) production by oxidizing H_(2)O in a portable photoelectrocatalysis(PEC)device.The obtained solution from this system is demonstrated for effective bactericidal activity against Staphylococcus aureus and Escherichia coli,while maintaining low toxicity toward hippocampal neuronal cells.The photoanode is achieved by Mo-doped BiVO4 films,which are subsequently loaded with cobalt-porphyrin(Co-py)molecules as a co-catalyst.As a result,the optimal performance for H_(2)O_(2) production rate was achieved at 8.4μmol h^(−1) cm^(−2),which is 1.8 times that of the pristine BiVO4 photoanode.Density functional theory(DFT)simulations reveal that the improved performance results from a 1.1 eV reduction in the energy of the rate-determining step of·OH adsorption by the optimal photoanode.This study demonstrates a PEC approach for promoting H_(2)O_(2) production by converting H_(2)O for antibacterial purposes,offering potential applications in conventionally controlling microenvironments for healthcare applications.
基金supported by the Financial Supports of the National Natural Science Foundation of China(Nos.51508056,52370030 and 42007352)the Chongqing Postgraduate Joint Training Base Project(No.JDLHPYJD2022005)the special fund of Henan Key Labora-tory of Water Pollution Control and Rehabilitation Technology(No.CJSZ2024001).
文摘This study developed a novel heterogeneous Vis-Photo+Fenton-like system by integrating visible-light-responsive Co_(3)O_(4)/TiO_(2) photocatalysis with peroxymonosulfate(PMS)activation for efficient atrazine(ATZ)degradation.The synergistic process achieved complete ATZ removal within 60 min under near-neutral pH(6.9),outperform-ing individual Fenton-like(39%)and photocatalytic(24%)processes.Key factors influencing the degradation efficiency included light sources(UV>visible),pH(optimal at 6.9),catalyst dosage(0.01 g Co_(3)O_(4)/TiO_(2)),and PMS:ATZ molar ratio(1:2).The system exhibited a synergistic coefficient of 5.03(degradation)and 1.97(miner-alization),attributed to enhanced radical generation and accelerated Co^(3+)/Co^(2+)redox cycling through photoin-duced electron transfer.Intermediate analysis revealed dealkylation,dechlorination,and oxidation pathways,with reduced toxicity of by-products(e.g.,CEAT,CIAT)confirmed by ecotoxicity assessments.The mineralization efficiency(Vis-Photo+Fenton-like)reached 83.1%,significantly higher than that of standalone processes(Fenton-like:43.2%;photocatalysis:30.5%).The catalyst demonstrated excellent stability(nearly 90%recov-ery,<1μg/L Co leaching)and practical applicability.This study provides an efficient,sludge-free,and solar-compatible strategy for eliminating persistent herbicides in water treatment.
基金supported by the National Key Research and Development Program of China(No.2021YFC2901100)the National Natural Science Foundation of China(No.22478425).
文摘Photocatalytic carbon dioxide(CO_(2))reduction offers an alternative strategy for converting CO_(2)into high-value added gaseous fuels,thereby paving the way for the development of clean and renewable energy.Metal-organic frameworks(MOFs),characterized by their highly porous structure,exceptional CO_(2)adsorption capacity,and tunable architecture,have emerged as promising candidates for photocatalytic CO_(2)reduction.This review systematically examines the recent advancement in MOFs-based photocatalysts for CO_(2)reduction to CO.It begins with the overview of the fundamental mechanisms and processes of MOFs towards photocatalytic CO_(2)reduction.Subsequently,common strategies for the modulation of MOFs-based photocatalysts are summarized,including metallic site modification,functionalized ligand incorporation,morphological control,defect engineering,and heterostructure construction.Notably,the review analyzes the critical factors contributing to the high selectivity of CO_(2)photoreduction to CO from both thermodynamic and kinetic perspectives.The conclusion addresses current challenges and future perspectives in designing highly efficient photocatalysts with abundant active sites,providing valuable insights for their continued development.
基金supported by the Program for New Century Talents in University(No.NCET-11-0951)from the Ministry of Education of ChinaKey Laboratory Project Fund of CAS(No.2005DP173065-2016-04).
文摘Photocatalytic oxygen reduction provides a sustainable method for on-site hydrogen peroxide(H_(2)O_(2))synthesis.However,most photocatalysts suffer from moderate kinetics due to sluggish electron transfer and inefficient oxygen adsorption and activation.Herein,sodium(Na)and potassium(K)are co-incorporated into graphitic carbon nitride(g-C_(3)N_(4))via a stepwise co-doping strategy combining sodium chloride-induced and molten salt-assisted polymerization.Experimental results and density functional theory calculations demonstrate that the synergistic interaction between intralayer Na+ions and interlayer K^(+)ions facilitates charge carrier separation and migration both within and between g-C_(3)N_(4)layers.Additionally,multiple heteroatom sites enhance surface charge polarization and introduce cyano groups,which synergistically promote oxygen molecule(O_(2))adsorption and elevate local proton coverage.Simultaneously,the energy barrier for H_(2)O_(2)desorption on the optimal photocatalyst(5Na/3.3K-CN)is lowered,thus improving H_(2)O_(2)production efficiency.Eventually,5Na/3.3K-CN exhibits an impressive H_(2)O_(2)yield of 2541.6μmol·g^(-1)·h^(-1) in an artificial reactor,which is 10.6 times higher than that of pure g-C_(3)N_(4)(240.2μmol·g^(-1)·h^(-1)).Under natural sunlight outdoors,5Na/3.3K-CN still maintains ultrahigh H_(2)O_(2)photosynthesis efficiency,achieving an H_(2)O_(2)photosynthesis rate of 2068.7μmol·g^(-1)·h^(-1).This work introduces a straightforward method to simultaneously optimize charge transfer and O_(2)activation for boosting H_(2)O_(2)photosynthesis,offering valuable insights toward the real-world deployment of g-C_(3)N_(4)-based photocatalysts in environmental protection and energy conversion.
基金supported by the Shaanxi Sanqin Scholars Innovation Team,the Science and Technology Project of Yan’an City(No.2023-CYL-193)the Key Science Research Plan of Department of Education in Shaanxi Province(No.23JS070)the Science Research Training Project(No.CLXZ2207).
文摘Photosynthesis is a promising method for H_(2)O_(2)production,but its application in pure water is limited by slow oxidation kinetics and rapid photocarrier recombination of photocatalysts.Herein,a novel defective carbon nitride photocatalyst(D-C3-xN4)containing the C vacancies and the frustrated Lewis pairs(B and N of cyano group)is designed for H_(2)O_(2)photosynthesis,and the role of C vacancies on the electron transfer mechanism during photocatalysis is systematically investigated.The D-C_(3-x)N_(4) exhibits a H_(2)O_(2)production rate of 140.1μmol·g^(-1)·h^(-1) in pure water,which is 87.6 times that of C_(3)N_(4).Such superior performance for H_(2)O_(2)photosynthesis is found to arise from the C vacancies and frustrated Lewis pairs(FLPs).The C vacancies have strong electron-trapping ability,which greatly enhances the separation of photocarriers.The C vacancies can also effectively reduce O_(2)to*OOH via a proton-coupled process,which significantly accelerates the O_(2)reduction kinetics.Meanwhile,the FLPs show an outstanding catalytic activity for H_(2)O oxidation.This study not only provides a new structure for highly active photocatalysts,but also deepens the understanding of the electron transfer mechanism of photocatalysts with trapped sites.
基金financially supported by the National Natural Science Foundation of China(No.22272159)the Chinese Academy of Sciences(No.KFJ-XCZX-202304).
文摘Single-atom catalysts based on graphitic carbon nitride(g-C_(3)N_(4))show high potential for hydrogen production photocatalytically.However,it is still a challenge to develop single-atom-based g-C_(3)N_(4)due to the complex synthesis procedures,limited active sites,and insufficient mechanistic understanding.Herein,a facile oxygen-tolerant synthesis strategy was developed,which utilizes the nitrogen-rich structure of g-C_(3)N_(4)to capture Fe single atoms from ammonium iron citrate,successfully constructing an efficient photocatalytic composite.The resulting Fe single-atom-modified g-C_(3)N_(4)catalyst exhibited highly improved light absorption,charge carrier separation,and a substantially enhanced rate of H_(2)production photocatalytically under visible light irradiation.Experimental results demonstrated that the optimal sample achieves a H_(2)production rate of 683μmol·h-1·g^(-1),representing a 425% enhancement compared to pristine g-C_(3)N_(4).This study presents a facile oxygen-tolerant approach for metal immobilization using metal-organic precursors,where the nitrogen-rich framework of g-C_(3)N_(4)effectively captures Fe atoms as singular site within the composite.The developed synthesis strategy provides new insights for designing high-performance single-atom photocatalytic materials,potentially advancing the application and development of photocatalysis.
基金financially supported by the National Basic Research Program of China(Nos.2022YFA1603701,2024YFC2310502,and 2024YFC2310503)the National Natural Science Foundation of China(Nos.22422403,82341044,and 22027810)+1 种基金the New Cornerstone Science Foundation(No.NCI202318)the Basic Science Center Project of the National Natural Science Foundation of China(No.22388101).
文摘Drug-resistant bacteria,using their dense cell membranes as strong barrier,significantly reduce the efficacy of conventional antibacterial treatments.Phototriggered 2D catalytic nanomaterials have emerged as promising candidates against drug-resistant bacteria by inducing membrane mechanical damage and generating reactive oxygen species(ROS).However,the practical antibacterial efficacy of typical 2D graphitic carbon nitride(g-C_(3)N_(4))is severely limited due to the low ROS production.Herein,we report an interfacial band-engineered lamellar heterojunctions(MnCN LHJs)through in situ Mn_(2)O_(3)growth on g-C_(3)N_(4).The charges generated in g-C_(3)N_(4)are stabilized by Mn_(2)O_(3),minimizing electron-hole recombination and boosting ROS production.Meanwhile,the photocatalytic effect of MnCN LHJs works synergistically with photothermal effects of Mn_(2)O_(3)to induce a robust“melee attack”against drug-resistant bacteria.High-resolution synchrotron radiation X-ray tomography directly visualized that MnCN LHJs possessed bacterial trapping capabilities,revealing their ability to induce mechanical damage to bacteria membrane for the first time.Additionally,MnCN LHJs can deplete endogenous glutathione,thereby enhancing ROS generation and weakening the bacterial antioxidant defense system.These combined effects achieve a remarkable bactericidal rate exceeding 98% against methicillin-resistant Staphylococcus aureus(MRSA).Notably,MnCN LHJs demonstrate prolonged retention at wound sites,helping to reduce inflammation and promote angiogenesis in infected wounds.This work not only advances interfacial band engineering approach to enhance the photocatalytic performance of g-C_(3)N_(4)but also underscores the significance of nanomaterial-bacteria interaction in design of next-generation antibacterial materials.
基金financially supported by the National Key R&D Program of China(No.2023YFB3810800)the National Natural Science Foundation of China(Nos.22579008,22502012,22301013,and 22272003)+3 种基金Key Project of the National Natural Science Foundation of China(No.21936001)R&D Program of Beijing Municipal Education Commission(No.KZ20231000506)Beijing Outstanding Young Scientists Program(No.BJJWZYJH01201910005017)the Project of Construction of Innovative Teams and Teacher Career Development for Universities and Colleges Under Beijing Municipality(No.11000024T000003219982).
文摘The integration of carbon dots(CDs)with graphitic carbon nitride(g-C_(3)N_(4))has emerged as a promising approach to enhance photocatalytic hydrogen(H_(2))evolution.Despite significant progress,critical challenges remain in achieving broad visiblelight absorption and suppressing charge recombination.In this work,we developed a series of photocatalysts through in situ embedding of red-emissive CDs(R-CDs)into g-C_(3)N_(4)(RCN)with precisely controlled loading amounts.Systematic characterization revealed that the R-CDs incorporation simultaneously addresses two fundamental limitations:(1)extending the light absorption edge to 800 nm,and(2)acting as an electron acceptor,facilitating charge separation.The optimized RCN composite demonstrates exceptional H_(2)evolution activity(1.87 mmol·g^(-1)·h^(-1),wavelength(λ)≥420 nm),representing a 3.3-fold enhancement over pristine g-C_(3)N_(4).Remarkably,the apparent quantum efficiency(AQE)reaches 9.1% at 420 nm,while maintaining measurable activity beyond 475 nm,where unmodified g-C_(3)N_(4)shows negligible response.This study provides fundamental insights into band structure engineering and charge carrier management through rational design of CDs-modified semiconductor heterostructures.
文摘Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-C_(3)N_(4) suffers from limited visible-light absorption and low charge-carrier mobility.In this study,a phosphorus-doped tubular carbon nitride(5P-TCN)was synthesized via a precursor self-assembly method using phosphoric acid and melamine as raw materials,eliminating the need for organic solvents or templates.The 5P-TCN catalyst demonstrated enhanced visible-light absorption,improved charge transfer capability,and a 5.25-fold increase in specific surface area(31.092 m^(2)/g),which provided abundant active sites to efficiently drive the PMS-assisted photocatalytic reaction.The 5P-TCN/vis/PMS system exhibited exceptional degradation performance for organic pollutants across a broad pH range(3–9),achieving over 92%degradation of Rhodamine B(RhB)within 15 min.Notably,the system retained>98%RhB degradation efficiency after three consecutive operational cycles,demonstrating robust operational stability and reusability.Moreover,key parameters influencing,active radi-cals,degradation pathways,and potential mechanisms for RhB degradation were systematically investigated.This work proposes a green and cost-effective strategy for developing high-efficiency photocatalysts,while demon-strating the exceptional capability of a PMS-assisted photocatalytic system for rapid degradation of RhB.
