In this study,melamine and cyanuric acid were used as precursors to form supramolecular crystals via hydrogen-bond-assisted self-assembly followed by hydrothermal treatment.Subsequent high-temperature calcination yiel...In this study,melamine and cyanuric acid were used as precursors to form supramolecular crystals via hydrogen-bond-assisted self-assembly followed by hydrothermal treatment.Subsequent high-temperature calcination yielded a novel brush-like three-dimensional carbon nitride.The brush-like 3D architecture was found to expose more accessible active sites,markedly accelerate electron transfer,and suppress the recombination of photogenerated charge carriers.The resulting superoxide(O_(2)^(-·))and hydroxyl(·OH)radicals generated via electron reduction were identified as the key reactive species in the photocatalytic process.Moreover,the surface of the brush-like structure is enriched with nitrogen vacancies,which enhance the catalyst’s ability to harvest visible light.The photocatalytic performance of the brush-like CNS-650 catalyst was evaluated for rhodamine B(RhB)degradation.Under red-light irradiation(660 nm),its degradation rate was 7.4 times higher than that of bulk CN.This work provides valuable insights into the design and application of efficient metal-free 3D photocatalysts.展开更多
Photocatalysis is one of the most promising technologies for solving environmental and energy problems,but current photocatalysts still suffer from low visible light utilization and insufficient photogenerated charge ...Photocatalysis is one of the most promising technologies for solving environmental and energy problems,but current photocatalysts still suffer from low visible light utilization and insufficient photogenerated charge separation efficiency.Therefore,in this work,D-A tubular materials with tubular carbon nitride(TCN)as electron donor(D)and 2-mercaptobenzothiazole(BZ)as electron acceptor(A)were constructed by molecular doping and modulation of the carbon nitride geometry.It was shown that the introduction of BZ could modulate the electronic structure of the catalyst,promote electron migration from TCN to BZ,and inhibit the recombination of photogenerated electrons and holes.Meanwhile,the ultra-thin tubular structure could expose more active sites.In addition,the adsorption of protons by BZ-TCN was further improved due to the modulation of the charge distribution between the components by the introduction of small molecules.Among them,the photocatalytic hydrogen production rate of BZ_(0.1)-TCN was twice that of TCN.The in-depth discussion of the components through theoretical calculations and characterization tests contributes to the understanding of the mechanism of photocatalytic hydrogen production.展开更多
Graphitic carbon nitride(g-CN)stands out as the most promising candidate for solar energy conversion owing to its easy preparation,metal-free nature,flexible molecular structure,moderate bandgap,and excellent thermal/...Graphitic carbon nitride(g-CN)stands out as the most promising candidate for solar energy conversion owing to its easy preparation,metal-free nature,flexible molecular structure,moderate bandgap,and excellent thermal/chemical stability.To enhance the performance of intrinsic g-CN,a supramolecular self-assembly strategy has been proposed to regulate the molecular structure of supramolecular precursors through non-covalent interactions across molecular building blocks,thereby optimizing the electronic structure of g-CN.This review provides a comprehensive overview of the recent progress in supramolecular self-assembly-derived graphitic carbon nitride(SM-CN)from both experimental and theoretical computational research in synthesis strategies,including synthesis methods and influencing factors,providing a theoretical foundation for the design of supramolecular assembly.It also discusses modification strategies,such as internal modification of the conjugated plane,interlayer optimization,and construction of heterointerfaces to improve the electronic structure of SM-CN owing to its unique layered structure.This review further summarizes the applications of SM-CN in environment and energy,including wastewater treatment,sterilization and disinfection/air purification,water splitting,H_(2)O_(2)production,organic synthesis/biomass conversion,CO_(2)reduction,photocatalytic coupling technology.Finally,perspectives and outlooks for the future development of SM-CN aim to inspire further innovation in the design and construction of high-performance SM-CN for broader applications.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
The two distinct types of composite materials(5%to 10%)were developed using recycled polyvinyl alcohol fiber(RPA),silicon nitride fiber(SN),and reduced carbon nanoparticles(RCN).Enhanced microstructural properties and...The two distinct types of composite materials(5%to 10%)were developed using recycled polyvinyl alcohol fiber(RPA),silicon nitride fiber(SN),and reduced carbon nanoparticles(RCN).Enhanced microstructural properties and mechanical strength were attained through the application of the 3-glycidoxypropyltrimethoxysilane coupling method.The combination of the resin-like properties of RPA-SN fiber resulted in the formation of robust outer strength and a high bonding structure.RPA-RCN composite materials with a weight percentage of 10%exhibited a tensile strength of 42 MPa.In contrast,RPA-SN-RCN composite materials containing 5%to 10%demonstrated enhanced tensile,bending,and hardness properties.Pyramid structures,solid structures,and crystal phases were formed using RCN particles.The resin and silane properties on hardness were gradually 14%increasing the outside region,whereas RPA-SN-RCN(10 wt%)on average hardness were attained at 86(Shore-D).The microstructures on RPA-RCN(5%to 10%)samples were observed solid structure,twin boundary’s structure and lattice structure.The tensile strength of RPA-SN-RCN(10%)was 67.3MPa,whereas the impact strength of RPA-RCN(10 wt%)was 53 J/mm2.The scanning electron microscopies(SEM)were used to investigate the microstructure of the RPA-SN-RCN(5%)and RPA-SN-RCN(10%)composite materials,respectively.展开更多
Unlocking the full potential of integrated photonics requires versatile,multi-functional devices that can adapt to diverse application demands.However,confronting this challenge with conventional singlefunction resona...Unlocking the full potential of integrated photonics requires versatile,multi-functional devices that can adapt to diverse application demands.However,confronting this challenge with conventional singlefunction resonators often results in cumbersome system designs.We present an elegant solution:a versatile and reconfigurable dual-polarization Si_(3)N_(4)microresonator that represents a new perspective in on-chip photonic designs.Our device can be dynamically reconfigured into three distinct topologies:a Möbius-like microcavity,a Fabry-Pérot resonator,and a microring resonator.This unprecedented functionality is enabled by a tunable balanced Mach-Zehnder interferometer that facilitates controllable mutual mode coupling of counterpropagating light using a single control knob.We experimentally demonstrate that the device not only supports polarization-diverse operation on a compact footprint but also gives rise to a wide variety of physical phenomena,including a standing wave cavity,a traveling wave cavity,free spectral range multiplication,and the photonic pinning effect.These behaviors are accurately modeled using the transfer matrix method and intuitively explained by the temporal coupled-mode theory.Our results underscore the potential for a chip-scale platform to realize reconfigurable reconstructive spectrometers and on-chip synthetic dimensions for topological physics.展开更多
High-entropy materials possess high hardness and strong wear resistance,yet the key bottleneck for their practical applications is the poor corrosion resistance in harsh environments.In this work,the high-entropy nitr...High-entropy materials possess high hardness and strong wear resistance,yet the key bottleneck for their practical applications is the poor corrosion resistance in harsh environments.In this work,the high-entropy nitride(HEN)coatings of(MoNbTaTiZr)1-x Nx(x=0-0.47)were fabricated using a hybrid di-rect current magnetron sputtering technique.The research focus was dedicated to the effect of nitrogen content on the microstructure,mechanical and electrochemical properties.The results showed that the as-deposited coatings exhibited a typical body-centered cubic(BCC)structure without nitrogen,while the amorphous matrix with face-centered cubic(FCC)nanocrystalline grain was observed at x=0.17.Further increasing x in the range of 0.35-0.47 caused the appearance of polycrystalline FCC phase in structure.Compared with the MoNbTaTiZr metallic coating,the coating containing nitrogen favored the high hard-ness around 13.7-32.4 GPa,accompanied by excellent tolerance both against elastic and plastic deforma-tion.Furthermore,such N-containing coatings yielded a low corrosion current density of about 10−8-10−7 A/cm^(2) and high electrochemical impedance of 10^(6)Ωcm^(2) in 3.5 wt.%NaCl solution,indicating the supe-rior corrosion resistance.The reason for the enhanced electrochemical behavior could be ascribed to the spontaneous formation of protective passive layers over the coating surface,which consisted of the domi-nated multi-elemental oxides in chemical stability.Particularly,noted that the(MoNbTaTiZr)_(0.83) N0.17 coat-ing displayed the highest hardness of 32.4±2.6 GPa and H/E ratio at 0.09,together with remarkable cor-rosion resistance,proposing the strongest capability for harsh-environmental applications required both good anti-wear and anti-corrosion performance.展开更多
Heterogeneous metal-catalyzed chemical conversions with a recyclable catalyst are very ideal and challenging for sustainable organic synthesis.A new bipyridyl-Mo(IV)-carbon nitride(CN-K/Mo-Bpy)was prepared by supporti...Heterogeneous metal-catalyzed chemical conversions with a recyclable catalyst are very ideal and challenging for sustainable organic synthesis.A new bipyridyl-Mo(IV)-carbon nitride(CN-K/Mo-Bpy)was prepared by supporting molybdenum complex on C_(3)N_(4)-K and characterized by FT-IR,XRD,SEM,XPS and ICP-OES.Heterogeneous CN–Mo-Bpy catalyst can be applied to the direct amination of nitroarenes and arylboronic acid,thus constructing various valuable diarylamines in high to excellent yields with a wide substrate scope and good functional group tolerance.It is worth noting that this heterogeneous catalyst has high chemical stability and can be recycled for at least five times without reducing its activity.展开更多
A series of divinylphenyl-acryloyl chloride copolymers(PDVB-co-PACl)is synthesized via atom transfer radical polymerization employing tert-butyl acrylate and divinylbenzene as monomers.PDVB-co-PACl is utilized to graf...A series of divinylphenyl-acryloyl chloride copolymers(PDVB-co-PACl)is synthesized via atom transfer radical polymerization employing tert-butyl acrylate and divinylbenzene as monomers.PDVB-co-PACl is utilized to graft on the surface of spherical aluminum nitride(AlN)to prepare functionalized AlN(AlN@PDVB-co-PACl).Polymethylhydrosiloxane(PMHS)is then used as the matrix to prepare thermally conductive AlN@PDVB-co-PACl/PMHS composites with AlN@PDVB-co-PACl as fillers through blending and curing.The grafting of PDVB-co-PACl synchronously enhances the hydrolysis resistance of AlN and its interfacial compatibility with PMHS matrix.When the molecular weight of PDVB-co-PACl is 5100 g mol^(-1)and the grafting density is 0.8 wt%,the composites containing 75 wt%of AlN@PDVB-co-PACl exhibit the optimal comprehensive performance.The thermal conductivity(λ)of the composite is 1.14 W m^(-1)K^(-1),which enhances by 20%and 420%compared to theλof simply physically blended AlN/PMHS composite and pure PMHS,respectively.Meanwhile,AlN@PDVB-co-PACl/PMHS composites display remarkable hydrothermal aging resistance by retaining 99.1%of itsλafter soaking in 90°C deionized water for 80 h,whereas theλof the blended AlN/PMHS composites decreases sharply to 93.7%.展开更多
Graphitic carbon nitride(g-C_(3)N_(4)),known for its green and abundant nature and composed of carbon and nitrogen in a two-dimensional structure,has emerged as a significant area of interest across various discipline...Graphitic carbon nitride(g-C_(3)N_(4)),known for its green and abundant nature and composed of carbon and nitrogen in a two-dimensional structure,has emerged as a significant area of interest across various disciplines,particularly in energy conversion and storage.Its recent demonstrations of high potential in supercapacitor applications mark it as a promising alternative to graphene within the realm of materials science.Numerous favorable features,such as chemical and thermal stability,abundant nitrogen content,eco-friendly attributes,and gentle conditions for synthesis,are shown.This review summarizes recent advancements in the use of g-C_(3)N_(4)and its composites as electrodes for supercapacitors,highlighting the advantages and issues associated with g-C_(3)N_(4)in these applications.This emphasizes situations where the composition of g-C_(3)N_(4)with other materials,such as metal oxides,metal chalcogenides,carbon materials,and conducting polymers,overcomes its limitations,leading to composite materials with improved functionalities.This review discusses the challenges that still need to be addressed and the possible future roles of g-C_(3)N_(4)in the research of advanced supercapacitor technology,such as battery-hybrid supercapacitors,flexible supercapacitors,and photo-supercapacitors.展开更多
Photocatalytic conversion of CO_(2) is pivotal for mitigating the global greenhouse effect and fostering sustainable energy development.Nowadays,polymeric carbon nitride(PCN)has gained widespread application in CO_(2)...Photocatalytic conversion of CO_(2) is pivotal for mitigating the global greenhouse effect and fostering sustainable energy development.Nowadays,polymeric carbon nitride(PCN)has gained widespread application in CO_(2) solar reduction due to its excellent visible light response,suitable conduction band position,and good cost-effectiveness.However,the amorphous nature and low conductivity of PCN limit its photocatalytic efficiency by leading to low carrier concentrations and facile electron–hole recombination during photocatalysis.Addressing this bottleneck,in this study,potassium-doped PCN(KPCN)/copper(Ⅱ)-complexed bipyridine hydroxyquinoline carboxylic acid(Cu(Ⅱ)(bpy)(H_(2)hqc))composite catalysts were synthesized through a multistep microwave heating process.In the composite,the formation of an S-scheme junction facilitates the enrichment of more negative electrons on the conduction band of KPCN via intermolecular electron–hole recombination between Cu(Ⅱ)(bpy)(H_(2)hqc)(CuPyQc)and KPCN,thereby promoting efficient photoreduction of CO_(2) to CO.Microwave heating enhances the amidation reaction between these two components,achieving the immobilization of homogeneous molecular catalysts and forming amidation chemical bonds that serve as key channels for the S-scheme charge transfer.This work not only presents a new PCN-based catalytic system for CO_(2) reduction applications,but also offers a novel microwave-practical approach for immobilizing homogeneous catalysts.展开更多
Thick electrodes can reduce the ratio of inactive constituents in a holistic energy storage system while improving energy and power densities.Unfortunately,traditional slurry-casting electrodes induce high-tortuous io...Thick electrodes can reduce the ratio of inactive constituents in a holistic energy storage system while improving energy and power densities.Unfortunately,traditional slurry-casting electrodes induce high-tortuous ionic diffusion routes that directly depress the capacitance with a thickening design.To overcome this,a novel 3D low-tortuosity,self-supporting,wood-structured ultrathick electrode(NiMoN@WC,a thickness of~1400 mm)with hierarchical porosity and artificial array-distributed small holes was constructed via anchoring bimetallic nitrides into the monolithic wood carbons.Accompanying the embedded NiMoN nanoclusters with well-designed geometric and electronic structure,the vertically low-tortuous channels,enlarged specific surface area and pore volume,superhydrophilic interface,and excellent charge conductivities,a superior capacitance of NiMoN@WC thick electrodes(~5350 mF cm^(-2)and 184.5 F g^(-1))is achieved without the structural deformation.In especial,monolithic wood carbons with gradient porous network not only function as the high-flux matrices to ameliorate the NiMoN loading via cell wall engineering but also allow fully-exposed electroactive substance and efficient current collection,thereby deliver an acceptable rate capability over 75%retention even at a high sweep rate of 20 mA cm^(-2).Additionally,an asymmetric NiMoN@WC//WC supercapacitor with an available working voltage of 1.0-1.8 V is assembled to demonstrate a maximum energy density of~2.04 mWh cm^(-2)(17.4 Wh kg^(-1))at a power density of 1620 mW cm^(-2),along with a decent long-term lifespan over 10,000 charging-discharging cycles.As a guideline,the rational design of wood ultrathick electrode with nanostructured transition metal nitrides sketch a promising blueprint for alleviating global energy scarcity while expanding carbon-neutral technologies.展开更多
Lowering the synthesis temperature of boron nitride nanotubes(BNNTs)is crucial for their development.The primary reason for adopting a high temperature is to enable the effective activation of highmelting-point solid ...Lowering the synthesis temperature of boron nitride nanotubes(BNNTs)is crucial for their development.The primary reason for adopting a high temperature is to enable the effective activation of highmelting-point solid boron.In this study,we developed a novel approach for efficiently activating boron by introducing alkali metal compounds into the conventional MgO–B system.This approach can be adopted to form various low-melting-point AM–Mg–B–O growth systems.These growth systems have improved catalytic capability and reactivity even under low-temperature conditions,facilitating the synthesis of BNNTs at temperatures as low as 850℃.In addition,molecular dynamics simulations based on density functional theory theoretically demonstrate that the systems maintain a liquid state at low temperatures and interact with N atoms to form BN chains.These findings offer novel insights into the design of boron activation and are expected to facilitate research on the low-temperature synthesis of BNNTs.展开更多
Exploration of stable metal single-site supported porous graphitic carbon nitride(PCN)nanostructures and the development of maximum atom utilization for enhanced photocatalytic oxidation of antibiotics remains a chall...Exploration of stable metal single-site supported porous graphitic carbon nitride(PCN)nanostructures and the development of maximum atom utilization for enhanced photocatalytic oxidation of antibiotics remains a challenge in current research.This work proposed a one-step thermal copolymerization to obtain Cu(Ⅰ)doping porous carbon nitride(CUCN)through a spontaneously reducing atmosphere by urea in a covered crucible.The obtained CUCN had crumpled ultrathin nanosheets and mesoporous structures,which possessed higher specific surface areas than PCN.From X-ray absorption near edge structure(XANES)and Fourier transform extended X-ray absorption fine structure(FT-EXAFS)spectra analysis,the Cu doping existed in the oxidation state of Cu(Ⅰ)as single atoms anchored on the 2D layers of CN through two N neighbors,thereby facilitating efficient pathways for the transfer of photoexcited charge carriers.Furthermore,the photoluminescence(PL)spectra,electrochemical impedance spectra(EIS)and transient photocurrent response test proved the improved separation and transfer of photoexcited charge carriers for Cu(Ⅰ)introduction.Consequently,the photocatalytic activity of CUCN was much better than that of PCN for antibiotics norfloxacin(NOR),with 4.7-fold higher degradation reaction rate constants.From species-trapping experiments and density function theory(DFT)calculations,the Cu single atoms in Cu-N_(2)served as catalytic sites that could accelerate charge transfer and facilitate the adsorption of molecular oxygen to produce active species.The stable Cu(Ⅰ)embedded in the layer structure led to the excellent recycling test and remained stable after four runs of degradation and even thermal regenerated treatment.The degradation paths of NOR by CUCN under visible light were also demonstrated.Our work sheds light on a sustainable and practical approach for achieving stable metal single-atom doping and enhancing photocatalytic degradation of aqueous pollutants.展开更多
Lithium-sulfur batteries are considered as one of the potential solutions as integrating renewable energy systems for large-scale energy storage because of their high theoretical energy density(2600 Wh·kg^(-1))an...Lithium-sulfur batteries are considered as one of the potential solutions as integrating renewable energy systems for large-scale energy storage because of their high theoretical energy density(2600 Wh·kg^(-1))and specific capacity(1675 mAh·g^(-1)).Currently,various strategies have been proposed to overcome the technical barriers,e.g.,“shuttle effect”,capacity decay and volumetric change,which impede the successful commercialization of lithium-sulfur batteries.This paper reviews the applications of metal nitrides as the cathode hosts for high-performance lithium-sulfur batteries,summa-rizes the design strategies of different host materials,and discusses the relationship between the properties of metal nitrides and their electrochemical performances.Finally,reasonable suggestions for the design and development of metal nitrides,along with ideas to promote future breakthroughs,are proposed.We hope that this review could attract more attention to metal nitrides and their derivatives,and further promote the electrochemical performance of lithium-sulfur batteries.展开更多
Graphitic carbon nitride(g-C_(3)N_(4))exhibits great mechanical as well as thermal characteristics,making it a valuable ma-terial for use in photoelectric conversion devices,an accelerator for synthesis of organic com...Graphitic carbon nitride(g-C_(3)N_(4))exhibits great mechanical as well as thermal characteristics,making it a valuable ma-terial for use in photoelectric conversion devices,an accelerator for synthesis of organic compounds,an electrolyte for fuel cell applications or power sources,and a hydrogen storage substance and a fluorescence detector.It is fabricated using dif-ferent methods,and there is a variety of morphologies and nanostructures such as zero to three dimensions that have been designed for different purposes.Ther e are many reports about g-C_(3)N_(4) in recent years,but a comprehensive review which covers nanostructure dimensions and their properties are missing.This review paper aims to give basic and comprehensive understanding of the photocatalytic and electrocatalytic usages of g-C_(3)N_(4).It highlights the recent progress of g-C_(3)N_(4) nano-structure designing by covering synthesis methods,dimensions,morphologies,applications and properties.Along with the summary,we will also discuss the challenges and prospects.Scientists,investigators,and engineers looking at g-C_(3)N_(4) nanostructures for a variety of applications might find our review paper to be a useful resource.展开更多
Elemental doping is an effective strategy for tuning the band structure of graphite carbon nitride(CN)to enhance its photocatalytic performance.In this study,sodium(Na)and oxygen(O)co-doped carbon nitride(Na/O-CN_(x),...Elemental doping is an effective strategy for tuning the band structure of graphite carbon nitride(CN)to enhance its photocatalytic performance.In this study,sodium(Na)and oxygen(O)co-doped carbon nitride(Na/O-CN_(x),x=1.0,2.0,3.0,4.0)was synthesized via solid-phase reaction of sodium citrate(NaCA)and pure CN powder in the Teflon-sealed autoclave under air conditions at 180℃.Surface area of Na/O-CN_(3.0) is measured to be 18.8 m^(2)/g,increasing by 60.7%compared to that of pure CN(11.7 m^(2)/g).Bandgap energy of Na/O-CN_(3.0) is determined to be 2.68 eV,marginally lower than that of pure CN(2.70 eV),thereby enhancing its capacity for sunlight absorption.Meanwhile,the incorporation of Na and O atoms into Na/O-CN_(x) is found to effectively reduce recombination rates of photogenerated electron-hole pairs.As a result,Na/O-CN_(x) samples exhibit markedly enhanced photocatalytic hydrogen evolution activity under visible light irradiation.Notably,the optimal Na/O-CN_(3.0) sample achieves a photocatalytic hydrogen production rate of 103.2μmol·g^(–1)·h^(–1),which is 8.2 times greater than that of pure CN(11.2μmol·g^(–1)·h^(–1)).Furthermore,a series of Na/O-CN_(x)-yO_(2)(y=0,20%,40%,60%,80%,100%)samples were prepared by modulating the oxygen content within reaction atmosphere.The catalytic performance evaluations reveal that the incorporation of both Na and O atoms in Na/O-CN_(3.0) enhances photocatalytic activity.This study also introduces novel methodologies for synthesis of metal atom-doped CN materials at lower temperature,highlighting the synergistic effect of Na and O atoms in photocatalytic hydrogen production of Na/O-CN_(x) samples.展开更多
Integrating photocatalysis technology with peroxymonosulfate oxidation possesses huge potential for degrading stubborn pollutant.Herein,a porous ultra-thin carbon nitride with C-defect O-doping and advanced n-π^(∗)tr...Integrating photocatalysis technology with peroxymonosulfate oxidation possesses huge potential for degrading stubborn pollutant.Herein,a porous ultra-thin carbon nitride with C-defect O-doping and advanced n-π^(∗)transition was customized by one-pot thermalinduced polymerization of molten urea assisted with paraformaldehyde.Via visible-light coupling peroxymonosulfate activation,the DCN-100 can completely photodegrade 2,4-dichlorophenol,and rate constant is 136.6 and 37.9 times that of CN and DCN-100 without peroxymonosulfate.The light-absorption of DCN-100 surpasses 550 nm,specific surface area rises from 45.03 to 98.58m^(2)/g,and charge behaviors are significantly improved.The effects of paraformaldehyde amount,PMS dosage,pH,2,4-dichlorophenol concentration,different water-body,wavelength and recycling times on photodegradation performance were explored in detail.Via capture experiments,ESR,LC-MS,Fukui-function,TEXT toxicity assessment and DFT theoretical calculation,themain active substances,degradation pathway,intermediate toxicity and enhanced activity mechanism of DCN-100 were clarified.The research provides a cost-effective,high-efficiency and environmental-friendly photocatalysts to activate peroxymonosulfate for water remediating.展开更多
Vanadium nitride(VN)is a promising pseudocapacitive material due to the high theoretical capacity,rapid redox Faradaic kinetics,and appropriate potential window.Although VN shows large pseudocapacitance in alkaline el...Vanadium nitride(VN)is a promising pseudocapacitive material due to the high theoretical capacity,rapid redox Faradaic kinetics,and appropriate potential window.Although VN shows large pseudocapacitance in alkaline electrolytes,the electrochemical instability and capacity degradation of VN electrode materials present significant challenges for practical applications.Herein,the capacitance decay mechanism of VN is investigated and a simple strategy to improve cycling stability of VN supercapacitor electrodes is proposed by introducing VO_(4)^(3-)anion in KOH electrolytes.Our results show that the VN electrode is electrochemical stabilization between-1.0and-0.4 V(vs.Hg/Hg O reference electrode)in 1.0 MKOH electrolyte,but demonstrates irreversible oxidation and fast capacitance decay in the potential range of-0.4 to0 V.In situ electrochemical measurements reveal that the capacitance decay of VN from-0.4 to 0 V is ascribed to the irreversible oxidation of vanadium(V)of N–V–O species by oxygen(O)of OH^(-).The as-generated oxidization species are subsequently dissolved into KOH electrolytes,thereby undermining the electrochemical stability of VN.However,this irreversible oxidation process could be hindered by introducing VO_(4)^(3-)in KOH electrolytes.A high volumetric specific capacitance of671.9 F.cm^(-3)(1 A.cm^(-3))and excellent cycling stability(120.3%over 1000 cycles)are achieved for VN nanorod electrode in KOH electrolytes containing VO_(4)^(3-).This study not only elucidates the failure mechanism of VN supercapacitor electrodes in alkaline electrolytes,but also provides new insights into enhancing pseudocapacitive energy storage of VN-based electrode materials.展开更多
基金Supported by the National Natural Science Foundation of China(Grant 22578376,52374283)the Natural Science Foundation of Jiangsu Province(Grant BK20240332)。
文摘In this study,melamine and cyanuric acid were used as precursors to form supramolecular crystals via hydrogen-bond-assisted self-assembly followed by hydrothermal treatment.Subsequent high-temperature calcination yielded a novel brush-like three-dimensional carbon nitride.The brush-like 3D architecture was found to expose more accessible active sites,markedly accelerate electron transfer,and suppress the recombination of photogenerated charge carriers.The resulting superoxide(O_(2)^(-·))and hydroxyl(·OH)radicals generated via electron reduction were identified as the key reactive species in the photocatalytic process.Moreover,the surface of the brush-like structure is enriched with nitrogen vacancies,which enhance the catalyst’s ability to harvest visible light.The photocatalytic performance of the brush-like CNS-650 catalyst was evaluated for rhodamine B(RhB)degradation.Under red-light irradiation(660 nm),its degradation rate was 7.4 times higher than that of bulk CN.This work provides valuable insights into the design and application of efficient metal-free 3D photocatalysts.
基金financially supported by the National Natural Science Foundation of China(No.22208129)2023 Jiangsu Province Large Scientific Instrument Open Sharing Autonomous Research Project(No.TC2023A033)。
文摘Photocatalysis is one of the most promising technologies for solving environmental and energy problems,but current photocatalysts still suffer from low visible light utilization and insufficient photogenerated charge separation efficiency.Therefore,in this work,D-A tubular materials with tubular carbon nitride(TCN)as electron donor(D)and 2-mercaptobenzothiazole(BZ)as electron acceptor(A)were constructed by molecular doping and modulation of the carbon nitride geometry.It was shown that the introduction of BZ could modulate the electronic structure of the catalyst,promote electron migration from TCN to BZ,and inhibit the recombination of photogenerated electrons and holes.Meanwhile,the ultra-thin tubular structure could expose more active sites.In addition,the adsorption of protons by BZ-TCN was further improved due to the modulation of the charge distribution between the components by the introduction of small molecules.Among them,the photocatalytic hydrogen production rate of BZ_(0.1)-TCN was twice that of TCN.The in-depth discussion of the components through theoretical calculations and characterization tests contributes to the understanding of the mechanism of photocatalytic hydrogen production.
基金supported by the National Natural Science Foundation of China(NSFC No.52271228)the Natural Science Foundation of Shaanxi Province(No.2023-JC-ZD-21)the Doctoral Dissertation Innovation Fund of Xi'an University of Technology(No.101-252072301)。
文摘Graphitic carbon nitride(g-CN)stands out as the most promising candidate for solar energy conversion owing to its easy preparation,metal-free nature,flexible molecular structure,moderate bandgap,and excellent thermal/chemical stability.To enhance the performance of intrinsic g-CN,a supramolecular self-assembly strategy has been proposed to regulate the molecular structure of supramolecular precursors through non-covalent interactions across molecular building blocks,thereby optimizing the electronic structure of g-CN.This review provides a comprehensive overview of the recent progress in supramolecular self-assembly-derived graphitic carbon nitride(SM-CN)from both experimental and theoretical computational research in synthesis strategies,including synthesis methods and influencing factors,providing a theoretical foundation for the design of supramolecular assembly.It also discusses modification strategies,such as internal modification of the conjugated plane,interlayer optimization,and construction of heterointerfaces to improve the electronic structure of SM-CN owing to its unique layered structure.This review further summarizes the applications of SM-CN in environment and energy,including wastewater treatment,sterilization and disinfection/air purification,water splitting,H_(2)O_(2)production,organic synthesis/biomass conversion,CO_(2)reduction,photocatalytic coupling technology.Finally,perspectives and outlooks for the future development of SM-CN aim to inspire further innovation in the design and construction of high-performance SM-CN for broader applications.
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.
基金the support provided by the Department of Mechanical Engineering,AAA college of Engineering and Technology,Sivakasi,Tamilnadu,India for facilitating the experimental and characterization facilities required to carry out this research work.
文摘The two distinct types of composite materials(5%to 10%)were developed using recycled polyvinyl alcohol fiber(RPA),silicon nitride fiber(SN),and reduced carbon nanoparticles(RCN).Enhanced microstructural properties and mechanical strength were attained through the application of the 3-glycidoxypropyltrimethoxysilane coupling method.The combination of the resin-like properties of RPA-SN fiber resulted in the formation of robust outer strength and a high bonding structure.RPA-RCN composite materials with a weight percentage of 10%exhibited a tensile strength of 42 MPa.In contrast,RPA-SN-RCN composite materials containing 5%to 10%demonstrated enhanced tensile,bending,and hardness properties.Pyramid structures,solid structures,and crystal phases were formed using RCN particles.The resin and silane properties on hardness were gradually 14%increasing the outside region,whereas RPA-SN-RCN(10 wt%)on average hardness were attained at 86(Shore-D).The microstructures on RPA-RCN(5%to 10%)samples were observed solid structure,twin boundary’s structure and lattice structure.The tensile strength of RPA-SN-RCN(10%)was 67.3MPa,whereas the impact strength of RPA-RCN(10 wt%)was 53 J/mm2.The scanning electron microscopies(SEM)were used to investigate the microstructure of the RPA-SN-RCN(5%)and RPA-SN-RCN(10%)composite materials,respectively.
基金supported by the National Natural Science Foundation of China(Grant Nos.62105061,12374301,and 62225404)the Jiangsu Provincial Frontier Technology Research and Development Program(Grant No.BF2024070)+1 种基金the National Key R&D Program of China(Grant No.2024YFA1210500)the Key Lab of Modern Optical Technologies of Education,Ministry of China,Soochow University。
文摘Unlocking the full potential of integrated photonics requires versatile,multi-functional devices that can adapt to diverse application demands.However,confronting this challenge with conventional singlefunction resonators often results in cumbersome system designs.We present an elegant solution:a versatile and reconfigurable dual-polarization Si_(3)N_(4)microresonator that represents a new perspective in on-chip photonic designs.Our device can be dynamically reconfigured into three distinct topologies:a Möbius-like microcavity,a Fabry-Pérot resonator,and a microring resonator.This unprecedented functionality is enabled by a tunable balanced Mach-Zehnder interferometer that facilitates controllable mutual mode coupling of counterpropagating light using a single control knob.We experimentally demonstrate that the device not only supports polarization-diverse operation on a compact footprint but also gives rise to a wide variety of physical phenomena,including a standing wave cavity,a traveling wave cavity,free spectral range multiplication,and the photonic pinning effect.These behaviors are accurately modeled using the transfer matrix method and intuitively explained by the temporal coupled-mode theory.Our results underscore the potential for a chip-scale platform to realize reconfigurable reconstructive spectrometers and on-chip synthetic dimensions for topological physics.
基金supported by the National Science Fund for Distinguished Young Scholars of China(No.52025014)Zhejiang Provincial Natural Science Foundation of China(Nos.LZJWY23E090001 and LD24E010003)the Natural Science Foundation of Ningbo(No.2022J305).
文摘High-entropy materials possess high hardness and strong wear resistance,yet the key bottleneck for their practical applications is the poor corrosion resistance in harsh environments.In this work,the high-entropy nitride(HEN)coatings of(MoNbTaTiZr)1-x Nx(x=0-0.47)were fabricated using a hybrid di-rect current magnetron sputtering technique.The research focus was dedicated to the effect of nitrogen content on the microstructure,mechanical and electrochemical properties.The results showed that the as-deposited coatings exhibited a typical body-centered cubic(BCC)structure without nitrogen,while the amorphous matrix with face-centered cubic(FCC)nanocrystalline grain was observed at x=0.17.Further increasing x in the range of 0.35-0.47 caused the appearance of polycrystalline FCC phase in structure.Compared with the MoNbTaTiZr metallic coating,the coating containing nitrogen favored the high hard-ness around 13.7-32.4 GPa,accompanied by excellent tolerance both against elastic and plastic deforma-tion.Furthermore,such N-containing coatings yielded a low corrosion current density of about 10−8-10−7 A/cm^(2) and high electrochemical impedance of 10^(6)Ωcm^(2) in 3.5 wt.%NaCl solution,indicating the supe-rior corrosion resistance.The reason for the enhanced electrochemical behavior could be ascribed to the spontaneous formation of protective passive layers over the coating surface,which consisted of the domi-nated multi-elemental oxides in chemical stability.Particularly,noted that the(MoNbTaTiZr)_(0.83) N0.17 coat-ing displayed the highest hardness of 32.4±2.6 GPa and H/E ratio at 0.09,together with remarkable cor-rosion resistance,proposing the strongest capability for harsh-environmental applications required both good anti-wear and anti-corrosion performance.
基金support for this work by Hebei Education Department(No.JZX2024004)Central Guidance on Local Science and Technology Development Fund of Hebei Province(No.236Z1404G)+3 种基金the National Natural Science Foundation of China(Nos.22301060 and 21272053)China Postdoctoral Science Foundation(No.2023M730914)the Natural Science Foundation of Hebei Province(Biopharmaceutical Joint Fund No.B2022206008)Project of Science and Technology Department of Hebei Province(No.22567622H)。
文摘Heterogeneous metal-catalyzed chemical conversions with a recyclable catalyst are very ideal and challenging for sustainable organic synthesis.A new bipyridyl-Mo(IV)-carbon nitride(CN-K/Mo-Bpy)was prepared by supporting molybdenum complex on C_(3)N_(4)-K and characterized by FT-IR,XRD,SEM,XPS and ICP-OES.Heterogeneous CN–Mo-Bpy catalyst can be applied to the direct amination of nitroarenes and arylboronic acid,thus constructing various valuable diarylamines in high to excellent yields with a wide substrate scope and good functional group tolerance.It is worth noting that this heterogeneous catalyst has high chemical stability and can be recycled for at least five times without reducing its activity.
基金support from the National Natural Science Foundation of China(52473083 and 52403112)the Technological Base Scientific Research Projects(Highly Thermal conductivity Nonmetal Materials),the Natural Science Basic Research Program of Shaanxi(2024JC-TBZC-04)+4 种基金the Shaanxi Province Key Research and Development Plan Project(2023-YBGY-461)the Innovation Capability Support Program of Shaanxi(2024RS-CXTD-57),the Natural Science Foundation of Chongqing,China(2023NSCQ-MSX2547)the Fundamental Research Funds for the Central Universities(D5000240077 and D5000240067)the Innovation Foundation for Doctor Dissertation of Northwestern Polytechnical University(CX2024094)the Analytical&Testing Center of Northwestern Polytechnical University for FT-IR,XRD and TEM tests performed in this work.
文摘A series of divinylphenyl-acryloyl chloride copolymers(PDVB-co-PACl)is synthesized via atom transfer radical polymerization employing tert-butyl acrylate and divinylbenzene as monomers.PDVB-co-PACl is utilized to graft on the surface of spherical aluminum nitride(AlN)to prepare functionalized AlN(AlN@PDVB-co-PACl).Polymethylhydrosiloxane(PMHS)is then used as the matrix to prepare thermally conductive AlN@PDVB-co-PACl/PMHS composites with AlN@PDVB-co-PACl as fillers through blending and curing.The grafting of PDVB-co-PACl synchronously enhances the hydrolysis resistance of AlN and its interfacial compatibility with PMHS matrix.When the molecular weight of PDVB-co-PACl is 5100 g mol^(-1)and the grafting density is 0.8 wt%,the composites containing 75 wt%of AlN@PDVB-co-PACl exhibit the optimal comprehensive performance.The thermal conductivity(λ)of the composite is 1.14 W m^(-1)K^(-1),which enhances by 20%and 420%compared to theλof simply physically blended AlN/PMHS composite and pure PMHS,respectively.Meanwhile,AlN@PDVB-co-PACl/PMHS composites display remarkable hydrothermal aging resistance by retaining 99.1%of itsλafter soaking in 90°C deionized water for 80 h,whereas theλof the blended AlN/PMHS composites decreases sharply to 93.7%.
基金financial support of the TMA pai scholarship from the Manipal Institute of Technology,Manipal Academy of Higher Education,Manipal,in achieving this milestone。
文摘Graphitic carbon nitride(g-C_(3)N_(4)),known for its green and abundant nature and composed of carbon and nitrogen in a two-dimensional structure,has emerged as a significant area of interest across various disciplines,particularly in energy conversion and storage.Its recent demonstrations of high potential in supercapacitor applications mark it as a promising alternative to graphene within the realm of materials science.Numerous favorable features,such as chemical and thermal stability,abundant nitrogen content,eco-friendly attributes,and gentle conditions for synthesis,are shown.This review summarizes recent advancements in the use of g-C_(3)N_(4)and its composites as electrodes for supercapacitors,highlighting the advantages and issues associated with g-C_(3)N_(4)in these applications.This emphasizes situations where the composition of g-C_(3)N_(4)with other materials,such as metal oxides,metal chalcogenides,carbon materials,and conducting polymers,overcomes its limitations,leading to composite materials with improved functionalities.This review discusses the challenges that still need to be addressed and the possible future roles of g-C_(3)N_(4)in the research of advanced supercapacitor technology,such as battery-hybrid supercapacitors,flexible supercapacitors,and photo-supercapacitors.
基金supported by the National Natural Science Foundation of China(Nos.22106105 and 22201180)the Innovation Program of Shanghai Municipal Education Commission(No.2019-01-07-00-E00015)+2 种基金Shanghai Science and Technology Innovation Program(No.21DZ1206300)the Central Local Science and Technology Development Guidance Fund(No.YDZX20213100003002)Shanghai Science and Technology Commission Program(No.20060502200).
文摘Photocatalytic conversion of CO_(2) is pivotal for mitigating the global greenhouse effect and fostering sustainable energy development.Nowadays,polymeric carbon nitride(PCN)has gained widespread application in CO_(2) solar reduction due to its excellent visible light response,suitable conduction band position,and good cost-effectiveness.However,the amorphous nature and low conductivity of PCN limit its photocatalytic efficiency by leading to low carrier concentrations and facile electron–hole recombination during photocatalysis.Addressing this bottleneck,in this study,potassium-doped PCN(KPCN)/copper(Ⅱ)-complexed bipyridine hydroxyquinoline carboxylic acid(Cu(Ⅱ)(bpy)(H_(2)hqc))composite catalysts were synthesized through a multistep microwave heating process.In the composite,the formation of an S-scheme junction facilitates the enrichment of more negative electrons on the conduction band of KPCN via intermolecular electron–hole recombination between Cu(Ⅱ)(bpy)(H_(2)hqc)(CuPyQc)and KPCN,thereby promoting efficient photoreduction of CO_(2) to CO.Microwave heating enhances the amidation reaction between these two components,achieving the immobilization of homogeneous molecular catalysts and forming amidation chemical bonds that serve as key channels for the S-scheme charge transfer.This work not only presents a new PCN-based catalytic system for CO_(2) reduction applications,but also offers a novel microwave-practical approach for immobilizing homogeneous catalysts.
基金support from the National Natural Science Foundation of China(32171728)Wuhan Knowledge Innovation Project(2022020801020312).
文摘Thick electrodes can reduce the ratio of inactive constituents in a holistic energy storage system while improving energy and power densities.Unfortunately,traditional slurry-casting electrodes induce high-tortuous ionic diffusion routes that directly depress the capacitance with a thickening design.To overcome this,a novel 3D low-tortuosity,self-supporting,wood-structured ultrathick electrode(NiMoN@WC,a thickness of~1400 mm)with hierarchical porosity and artificial array-distributed small holes was constructed via anchoring bimetallic nitrides into the monolithic wood carbons.Accompanying the embedded NiMoN nanoclusters with well-designed geometric and electronic structure,the vertically low-tortuous channels,enlarged specific surface area and pore volume,superhydrophilic interface,and excellent charge conductivities,a superior capacitance of NiMoN@WC thick electrodes(~5350 mF cm^(-2)and 184.5 F g^(-1))is achieved without the structural deformation.In especial,monolithic wood carbons with gradient porous network not only function as the high-flux matrices to ameliorate the NiMoN loading via cell wall engineering but also allow fully-exposed electroactive substance and efficient current collection,thereby deliver an acceptable rate capability over 75%retention even at a high sweep rate of 20 mA cm^(-2).Additionally,an asymmetric NiMoN@WC//WC supercapacitor with an available working voltage of 1.0-1.8 V is assembled to demonstrate a maximum energy density of~2.04 mWh cm^(-2)(17.4 Wh kg^(-1))at a power density of 1620 mW cm^(-2),along with a decent long-term lifespan over 10,000 charging-discharging cycles.As a guideline,the rational design of wood ultrathick electrode with nanostructured transition metal nitrides sketch a promising blueprint for alleviating global energy scarcity while expanding carbon-neutral technologies.
基金supported by the National Natural Science Foundation of China(No.51972162)the Fundamental Research Funds for the Central Universities(No.2024300440).
文摘Lowering the synthesis temperature of boron nitride nanotubes(BNNTs)is crucial for their development.The primary reason for adopting a high temperature is to enable the effective activation of highmelting-point solid boron.In this study,we developed a novel approach for efficiently activating boron by introducing alkali metal compounds into the conventional MgO–B system.This approach can be adopted to form various low-melting-point AM–Mg–B–O growth systems.These growth systems have improved catalytic capability and reactivity even under low-temperature conditions,facilitating the synthesis of BNNTs at temperatures as low as 850℃.In addition,molecular dynamics simulations based on density functional theory theoretically demonstrate that the systems maintain a liquid state at low temperatures and interact with N atoms to form BN chains.These findings offer novel insights into the design of boron activation and are expected to facilitate research on the low-temperature synthesis of BNNTs.
基金supported by the National Natural Science Foundation of China(Nos.52070103 and 22102102)Zhejiang Provincial Natural Science Foundation of China(Nos.LY21E090004 and LQ22B050004)+1 种基金Ningbo Public Welfare Science and Technology Program(No.2021S025)Ningbo Youth Leading Talent Project(No.2024QL038).
文摘Exploration of stable metal single-site supported porous graphitic carbon nitride(PCN)nanostructures and the development of maximum atom utilization for enhanced photocatalytic oxidation of antibiotics remains a challenge in current research.This work proposed a one-step thermal copolymerization to obtain Cu(Ⅰ)doping porous carbon nitride(CUCN)through a spontaneously reducing atmosphere by urea in a covered crucible.The obtained CUCN had crumpled ultrathin nanosheets and mesoporous structures,which possessed higher specific surface areas than PCN.From X-ray absorption near edge structure(XANES)and Fourier transform extended X-ray absorption fine structure(FT-EXAFS)spectra analysis,the Cu doping existed in the oxidation state of Cu(Ⅰ)as single atoms anchored on the 2D layers of CN through two N neighbors,thereby facilitating efficient pathways for the transfer of photoexcited charge carriers.Furthermore,the photoluminescence(PL)spectra,electrochemical impedance spectra(EIS)and transient photocurrent response test proved the improved separation and transfer of photoexcited charge carriers for Cu(Ⅰ)introduction.Consequently,the photocatalytic activity of CUCN was much better than that of PCN for antibiotics norfloxacin(NOR),with 4.7-fold higher degradation reaction rate constants.From species-trapping experiments and density function theory(DFT)calculations,the Cu single atoms in Cu-N_(2)served as catalytic sites that could accelerate charge transfer and facilitate the adsorption of molecular oxygen to produce active species.The stable Cu(Ⅰ)embedded in the layer structure led to the excellent recycling test and remained stable after four runs of degradation and even thermal regenerated treatment.The degradation paths of NOR by CUCN under visible light were also demonstrated.Our work sheds light on a sustainable and practical approach for achieving stable metal single-atom doping and enhancing photocatalytic degradation of aqueous pollutants.
文摘Lithium-sulfur batteries are considered as one of the potential solutions as integrating renewable energy systems for large-scale energy storage because of their high theoretical energy density(2600 Wh·kg^(-1))and specific capacity(1675 mAh·g^(-1)).Currently,various strategies have been proposed to overcome the technical barriers,e.g.,“shuttle effect”,capacity decay and volumetric change,which impede the successful commercialization of lithium-sulfur batteries.This paper reviews the applications of metal nitrides as the cathode hosts for high-performance lithium-sulfur batteries,summa-rizes the design strategies of different host materials,and discusses the relationship between the properties of metal nitrides and their electrochemical performances.Finally,reasonable suggestions for the design and development of metal nitrides,along with ideas to promote future breakthroughs,are proposed.We hope that this review could attract more attention to metal nitrides and their derivatives,and further promote the electrochemical performance of lithium-sulfur batteries.
基金M Tahir is funded by EU H2020 Marie Skłodows-ka-Curie Fellowship(1439425).
文摘Graphitic carbon nitride(g-C_(3)N_(4))exhibits great mechanical as well as thermal characteristics,making it a valuable ma-terial for use in photoelectric conversion devices,an accelerator for synthesis of organic compounds,an electrolyte for fuel cell applications or power sources,and a hydrogen storage substance and a fluorescence detector.It is fabricated using dif-ferent methods,and there is a variety of morphologies and nanostructures such as zero to three dimensions that have been designed for different purposes.Ther e are many reports about g-C_(3)N_(4) in recent years,but a comprehensive review which covers nanostructure dimensions and their properties are missing.This review paper aims to give basic and comprehensive understanding of the photocatalytic and electrocatalytic usages of g-C_(3)N_(4).It highlights the recent progress of g-C_(3)N_(4) nano-structure designing by covering synthesis methods,dimensions,morphologies,applications and properties.Along with the summary,we will also discuss the challenges and prospects.Scientists,investigators,and engineers looking at g-C_(3)N_(4) nanostructures for a variety of applications might find our review paper to be a useful resource.
基金National Natural Science Foundation of China(21806023)Natural Science Foundation of Hunan Province(2021JJ40199)+2 种基金Education Department Foundation of Hunan Province(20C0813)Hunan University of Science and Technology Fundamental Research FundsPostgraduate Scientific Research Innovation Project of Hunan Province(CX20240877)。
文摘Elemental doping is an effective strategy for tuning the band structure of graphite carbon nitride(CN)to enhance its photocatalytic performance.In this study,sodium(Na)and oxygen(O)co-doped carbon nitride(Na/O-CN_(x),x=1.0,2.0,3.0,4.0)was synthesized via solid-phase reaction of sodium citrate(NaCA)and pure CN powder in the Teflon-sealed autoclave under air conditions at 180℃.Surface area of Na/O-CN_(3.0) is measured to be 18.8 m^(2)/g,increasing by 60.7%compared to that of pure CN(11.7 m^(2)/g).Bandgap energy of Na/O-CN_(3.0) is determined to be 2.68 eV,marginally lower than that of pure CN(2.70 eV),thereby enhancing its capacity for sunlight absorption.Meanwhile,the incorporation of Na and O atoms into Na/O-CN_(x) is found to effectively reduce recombination rates of photogenerated electron-hole pairs.As a result,Na/O-CN_(x) samples exhibit markedly enhanced photocatalytic hydrogen evolution activity under visible light irradiation.Notably,the optimal Na/O-CN_(3.0) sample achieves a photocatalytic hydrogen production rate of 103.2μmol·g^(–1)·h^(–1),which is 8.2 times greater than that of pure CN(11.2μmol·g^(–1)·h^(–1)).Furthermore,a series of Na/O-CN_(x)-yO_(2)(y=0,20%,40%,60%,80%,100%)samples were prepared by modulating the oxygen content within reaction atmosphere.The catalytic performance evaluations reveal that the incorporation of both Na and O atoms in Na/O-CN_(3.0) enhances photocatalytic activity.This study also introduces novel methodologies for synthesis of metal atom-doped CN materials at lower temperature,highlighting the synergistic effect of Na and O atoms in photocatalytic hydrogen production of Na/O-CN_(x) samples.
基金supported by the Natural Science Foundation Project of Jilin Province(Nos.20230101297JC,YDZJ202201ZYTS347,YDZJ202101ZYTS073,20210101117JC,YDZJ202201ZYTS349,YDZJ202102CXJD049)the National Natural Science Foundation(22004047)+4 种基金China Postdoctoral Science Foundation(No.2023M731299)the Project of Jilin Province Development and Reform Commission(Nos.2023C032-5,2023C032-4,2023C032-2)the Project of Human Resources and Social Security Department of Jilin Province(No.2023337)the National College students’innovation and entrepreneurship training program(No.202310203008)the Project of Education Department of Jilin Province(Nos.JJKH20220429KJ,JJKH20210460KJ).
文摘Integrating photocatalysis technology with peroxymonosulfate oxidation possesses huge potential for degrading stubborn pollutant.Herein,a porous ultra-thin carbon nitride with C-defect O-doping and advanced n-π^(∗)transition was customized by one-pot thermalinduced polymerization of molten urea assisted with paraformaldehyde.Via visible-light coupling peroxymonosulfate activation,the DCN-100 can completely photodegrade 2,4-dichlorophenol,and rate constant is 136.6 and 37.9 times that of CN and DCN-100 without peroxymonosulfate.The light-absorption of DCN-100 surpasses 550 nm,specific surface area rises from 45.03 to 98.58m^(2)/g,and charge behaviors are significantly improved.The effects of paraformaldehyde amount,PMS dosage,pH,2,4-dichlorophenol concentration,different water-body,wavelength and recycling times on photodegradation performance were explored in detail.Via capture experiments,ESR,LC-MS,Fukui-function,TEXT toxicity assessment and DFT theoretical calculation,themain active substances,degradation pathway,intermediate toxicity and enhanced activity mechanism of DCN-100 were clarified.The research provides a cost-effective,high-efficiency and environmental-friendly photocatalysts to activate peroxymonosulfate for water remediating.
基金financially supported by the National Natural Science Foundation of China(No.U2004210)Application Foundation Frontier Project of Wuhan Science and Technology Program(No.2020010601012199)City University of Hong Kong Strategic Research Grant,Hong Kong,China(No.7005505)。
文摘Vanadium nitride(VN)is a promising pseudocapacitive material due to the high theoretical capacity,rapid redox Faradaic kinetics,and appropriate potential window.Although VN shows large pseudocapacitance in alkaline electrolytes,the electrochemical instability and capacity degradation of VN electrode materials present significant challenges for practical applications.Herein,the capacitance decay mechanism of VN is investigated and a simple strategy to improve cycling stability of VN supercapacitor electrodes is proposed by introducing VO_(4)^(3-)anion in KOH electrolytes.Our results show that the VN electrode is electrochemical stabilization between-1.0and-0.4 V(vs.Hg/Hg O reference electrode)in 1.0 MKOH electrolyte,but demonstrates irreversible oxidation and fast capacitance decay in the potential range of-0.4 to0 V.In situ electrochemical measurements reveal that the capacitance decay of VN from-0.4 to 0 V is ascribed to the irreversible oxidation of vanadium(V)of N–V–O species by oxygen(O)of OH^(-).The as-generated oxidization species are subsequently dissolved into KOH electrolytes,thereby undermining the electrochemical stability of VN.However,this irreversible oxidation process could be hindered by introducing VO_(4)^(3-)in KOH electrolytes.A high volumetric specific capacitance of671.9 F.cm^(-3)(1 A.cm^(-3))and excellent cycling stability(120.3%over 1000 cycles)are achieved for VN nanorod electrode in KOH electrolytes containing VO_(4)^(3-).This study not only elucidates the failure mechanism of VN supercapacitor electrodes in alkaline electrolytes,but also provides new insights into enhancing pseudocapacitive energy storage of VN-based electrode materials.
