Zinc-ion hybrid supercapacitors(ZHSCs)have enormous potential for future applications in electric vehi-cles,portable/wearable electronic gadgets,etc.However,to accelerate ZHSC technology towards market applications,it...Zinc-ion hybrid supercapacitors(ZHSCs)have enormous potential for future applications in electric vehi-cles,portable/wearable electronic gadgets,etc.However,to accelerate ZHSC technology towards market applications,it is necessary to overcome research challenges such as Zn dendrites,low Zn utilization,and all-climate adaptability,as well as to streamline the device assembly process.In this study,we propose a new strategy for the facile construction of ZHSC via two porous carbon fabrics and a Zn plating solution.The cathode and current collector of the device are both porous graphitized carbon fabric(PGCF)pre-pared by high-temperature activation of K2 FeO_(4),and the Li_(2)ZnCl_(4)·9H_(2)O electrolyte is verified to possess excellent Zn plating/stripping efficiency and inhibition of Zn dendrite growth in a Zn-Zn symmetric cell model.As a result,the assembled ZHSC has the maximum energy density of 2.02 mWh cm^(−2)and the highest power density of 11.47 mW cm^(−2),and it can operate for 30,000 cycles without capacity degrada-tion.Furthermore,the destruction of the hydrogen bonding network by the high concentration of Cl−at low temperatures endows it with low freezing point properties and excellent ionic activity at low tem-peratures.The device also operated reliably at-60℃,with a maximum areal capacity of 1.15 mAh cm^(−2).This research offers new findings and insights for the development of high-performance ultra-cryogenic ZHSC devices.展开更多
Potassium-ion batteries(KIBs)have great potential for applications in large-scale energy storage devices.However,the larger radius of K+leads to sluggish kinetics and inferior cycling performance,severely restricting ...Potassium-ion batteries(KIBs)have great potential for applications in large-scale energy storage devices.However,the larger radius of K+leads to sluggish kinetics and inferior cycling performance,severely restricting its practical applicability.Herein,we propose a rational strategy involving a Prussian blue analogue-derived graphitized carbon anode with fast and durable potassium storage capability,which is constructed by encapsulating cobalt nanoparticles in nitrogen-doped graphitized carbon(Co-NC).Both experimental and theoretical results show that N-doping effectively promotes the uniform dispersion of cobalt nanoparticles in the carbon matrix through Co-N bonds.Moreover,the cobalt nanoparticles and strong Co-N bonds synergistically form a threedimensional conductive network,increase the number of adsorption sites,and reduce the diffusion energy barrier,thereby facilitating the adsorption and the diffusion kinetics.These multiple effects lead to enhanced reversible capacities of 305 and 208.6 mAh g^−1 after 100 and 300 cycles at 0.05 and 0.1 A g^−1,respectively,demonstrating the applicability of the Co-NC anode for KIBs.展开更多
Cocatalysts play important roles in improving the activity and stability of most photocatalysts.It is of great significance to develop economical,efficient and stable cocatalysts.Herein,using Na2CoFe(CN)6 complex as p...Cocatalysts play important roles in improving the activity and stability of most photocatalysts.It is of great significance to develop economical,efficient and stable cocatalysts.Herein,using Na2CoFe(CN)6 complex as precursor,a novel noble-metal-free FeCo@NGC cocatalyst(nano-FeCo alloy@N-doped graphitized carbon) is fabricated by a simple pyrolysis method.Coupling with g-C3 N4, the optimal FeCo@NGC/g-C3N4 receives a boosted visible light driven photocatalytic H2 evolution rate of 42.2 μmol h-1, which is even higher than that of 1.0 wt% Pt modified g-C3N4 photocatalyst.Based on the results of density functional theory(DFT) calculations and practical experiment measurements,such outstanding photocatalytic performance of FeCo@NGC/g-C3N4 is mainly attributed to two aspects.One is the accelerated charge transfer behavior,induced by a photogene rated electrons secondary transfer performance on the surface of FeCo alloy nanoparticles.The other is related to the adjustment of H adsorption energy(approaching the standard hydrogen electrode potential) by the presence of external NGC thin layer.Both factors play key roles in the H2 evolution reaction.Such outstanding performance highlights an enormous potential of developing noble-metal-free bimetallic nano-alloy as inexpensive and efficient cocatalysts for solar applications.展开更多
Exploring nonprecious electrocatalysts for water splitting with high efficiency and durability is critically important.Herein,bimetallic phosphides are encapsulated into graphitized carbon to construct a C@NiCoP compo...Exploring nonprecious electrocatalysts for water splitting with high efficiency and durability is critically important.Herein,bimetallic phosphides are encapsulated into graphitized carbon to construct a C@NiCoP composite nanoarray using bimetallic metal-organic framework(MOF) as a self-sacrificial template.The resulting C@NiCoP exhibits superior performance for pH-universal electrocatalytic hydrogen evolution reaction(HER),particularly representing a low overpotential of 46.3 mV at 10 mA cm^(-2) and Tafel slope of 44.1 mV dec^(-1) in alkaline media.The structural characterizations combined with theoretical calculation demonstrate that tailored electronic structure from bimetal atoms and the synergistic effect with graphitized carbon layer could jointly optimize the adsorption ability of hydrogen on active sites in HER process,and enhance the electrical conductivity as well.In addition,the carbon layer served as a protecting shell also prevents highly dispersed NiCoP components from agglomeration and/or loss in harsh media,finally improving the durability.This work thus provides a new insight into optimizing activity and stability of pH-universal electrocatalysts by the nanostructural design and electronic structure modulation.展开更多
A novel chromatography stationary phase with a quasi-graphitized carbon modified shell has been developed. Coal pitch was directly carbonized on the surface of porous silica with in-situ carbonization. The carbonized ...A novel chromatography stationary phase with a quasi-graphitized carbon modified shell has been developed. Coal pitch was directly carbonized on the surface of porous silica with in-situ carbonization. The carbonized coal pitch coating exhibits some degree of graphitization with a 78 nm-thick layer on the surface of silica and a 0.5 nm-thick layer on the inner surface of the mesopores. Based on the special structure of the graphitized carbon coating, the novel stationary phase can provide multiple interactions such as hydrophobic interaction, π-π interaction and dipole-dipole interaction. The novel composite material exhibited unique separation selectivity and excellent separation efficiency for polar compounds, including imidazoles, nucleosides and pesticides. Besides, the packed column also exhibited great repeatability with the RSDs of the retention time of nucleosides between 0.07%-0.50%(n = 5). Finally, satisfied result was achieved in the separation of fullerenes on the new column, suggesting the great potential in the industrial-scale purification of fullerenes.展开更多
Due to inefficient diagnostic methods,inflammatory bowel disease(IBD)normally progresses into severe complications including cancer.Highly efficient extraction and identification of metabolic fingerprints are of signi...Due to inefficient diagnostic methods,inflammatory bowel disease(IBD)normally progresses into severe complications including cancer.Highly efficient extraction and identification of metabolic fingerprints are of significance for disease surveillance.In this work,we synthesized a layered titania nanosheet doped with graphitized carbon(2D-GC-mTNS)through a simple one-step assembly process for assisting laser desorption ionization mass spectrometry(LDI-MS)for metabolite analysis.Based on the synergistic effect of graphitized carbon and mesoporous titania,2D-GC-mTNS exhibits good extraction ability including high sensitivity(<1 fmolμL−1)and great repeatability toward metabolites.A total of 996 fingerprint spectra were collected from hundreds of native urine samples(including IBD patients and healthy controls),each of which contained 1220 m/z metabolite features.Diagnostic model was further established for precise discrimination of patients from healthy controls,with high area under the curve value of 0.972 and 0.981 toward discovery cohort and validation cohort,respectively.The 2D-GC-mTNS promotes LDI-MS to be close to clinical application,with rapid speed,minimum sample consumption and free of sample pretreatment.展开更多
Graphitized spent carbon cathode(SCC)is a hazardous solid waste generated in the aluminum electrolysis process.In this study,a flotation-acid leaching process is proposed for the purification of graphitized SCC,and th...Graphitized spent carbon cathode(SCC)is a hazardous solid waste generated in the aluminum electrolysis process.In this study,a flotation-acid leaching process is proposed for the purification of graphitized SCC,and the use of the purified SCC as an anode material for lithium-ion batteries is explored.The flotation and acid leaching processes were separately optimized through one-way experiments.The maximum SCC carbon content(93wt%)was achieved at a 90%proportion of−200-mesh flotation particle size,a slurry concentration of 10wt%,a rotation speed of 1600 r/min,and an inflatable capacity of 0.2 m^(3)/h(referred to as FSCC).In the subsequent acid leaching process,the SCC carbon content reached 99.58wt%at a leaching concentration of 5 mol/L,a leaching time of 100 min,a leaching temperature of 85°C,and an HCl/FSCC volume ratio of 5:1.The purified graphitized SCC(referred to as FSCC-CL)was utilized as an anode material,and it exhibited an initial capacity of 348.2 mAh/g at 0.1 C and a reversible capacity of 347.8 mAh/g after 100 cycles.Moreover,compared with commercial graphite,FSCC-CL exhibited better reversibility and cycle stability.Thus,purified SCC is an important candidate for anode material,and the flotation-acid leaching purification method is suitable for the resourceful recycling of SCC.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
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
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
The advancement of planar micro-supercapacitors(PMSCs)for micro-electromechanical systems(MEMS)has been significantly hindered by the challenge of achieving high energy and power densities.This study addresses this is...The advancement of planar micro-supercapacitors(PMSCs)for micro-electromechanical systems(MEMS)has been significantly hindered by the challenge of achieving high energy and power densities.This study addresses this issue by leveraging screen-printing technology to fabricate high-performance PMSCs using innovative composite ink.The ink,a synergistic blend of few-layer graphene(Gt),carbon black(CB),and NiCo_(2)O_(4),was meticulously mixed to form a conductive and robust coating that enhanced the capacitive performance of the PMSCs.The optimized ink formulation and printing process result in a micro-supercapacitor with an exceptional areal capacitance of 18.95 mF/cm^(2)and an areal energy density of 2.63μW·h/cm^(2)at a current density of 0.05 mA/cm^(2),along with an areal power density of 0.025 mW/cm^(2).The devices demonstrated impressive durability with a capacitance retention rate of 94.7%after a stringent 20000-cycle test,demonstrating their potential for long-term applications.Moreover,the PMSCs displayed excellent mechanical flexibility,with a capacitance decrease of only 3.43%after 5000 bending cycles,highlighting their suitability for flexible electronic devices.The ease of integrating these PMSCs into series and parallel configurations for customized power further underscores their practicality for integrated power supply solutions in various technologies.展开更多
The rapid emergence of drug-resistant bacterial strains undermines the efficacy of conventional antibiotics,necessitating the development of alternative therapies.Antimicrobial photodynamic therapy(PDT)is a promising ...The rapid emergence of drug-resistant bacterial strains undermines the efficacy of conventional antibiotics,necessitating the development of alternative therapies.Antimicrobial photodynamic therapy(PDT)is a promising approach,but its effectiveness is often limited by the suboptimal photocatalytic activity of photosensitizers.In this study,we introduce a novel photoresponsive carbon-based antibacterial agent,Ce6/g-C_(3)N_(4),which combines the photocatalytic properties of graphite-phase carbon nitride(g-C_(3)N_(4))with the photodynamic attributes of chlorin e6(Ce6).This agent,with an average particle size of 250.7 nm,demonstrates significantly enhanced photocatalytic activity.Additionally,the strong affinity of Ce6/g-C_(3)N_(4)for bacteria and efficient delivery of Ce6 result in an inhibition rate exceeding 99%against Gram-positive bacteria and excellent biofilm eradication under light irradiation.In vivo experiments reveal that Ce6/gC_(3)N_(4)effectively inhibits bacterial growth on wounds,and promotes wound healing post-light treatment,while maintaining good biocompatibility.Overall,the Ce6/g-C_(3)N_(4)antibacterial agent synergizes photodynamic and photocatalytic mechanisms,offering a new avenue for the photo-mediated,multi-strategic treatment of bacterial infections and wound healing.展开更多
Graphitic carbon nitride(g-C_(3)N_(4))has garnered significant attention due to its remarkable advantages such as lightweight,exceptional chemical stability and defect-rich surface.Nevertheless,its inadequate electric...Graphitic carbon nitride(g-C_(3)N_(4))has garnered significant attention due to its remarkable advantages such as lightweight,exceptional chemical stability and defect-rich surface.Nevertheless,its inadequate electrical conductivity and impedance matching hindered the practical implementation in the electromagnetic wave absorption(EMWA)field.To address these challenges,we developed a composites system of carbon spheres/g-C_(3)N_(4)(CCN)through a supramolecular self-assembly strategy,subsequently integrated with reduced graphene oxide(RGO)via a water bath method.Systematic investigation revealed that the EMWA performance of CCN/RGO composites exhibited a distinct dependence(a trend of first increasing and then decreasing)on RGO content.Especially,when the mass ratio of RGO to CCN was 20%,the CCN/RGO composite brought a minimum reflection loss value of-45.40 dB at 13.44 GHz and a broad effective absorbing bandwidth of 6.32 GHz at 2.19 mm.First-principles calculations based on density functional theory suggested that the constructed heterostructure effectively facilitated electron mobility and charge redistribution,boosting both conductive loss and polarization loss mechanisms.The exceptional absorption performance was ascribed to the synergistic effects of conductive loss,relaxation loss,and suitable impedance matching.As a results,this work provided a rational design strategy for high-performance g-C_(3)N_(4)-based EMWA materials.展开更多
Rational design of defected carbons adjacent to nitrogen(N)dopants is a fascinating but challenging approach for enhancing the catalytic performance of N-doped carbon.Meanwhile,the combined effect of heteroatom doping...Rational design of defected carbons adjacent to nitrogen(N)dopants is a fascinating but challenging approach for enhancing the catalytic performance of N-doped carbon.Meanwhile,the combined effect of heteroatom doping and defect engineering can efficiently increase the oxygen reduction reaction(ORR)ability of inactive carbons through charge redistribution.Herein,we report that an enhanced built-in electric field caused by the combined effect of N-doping and carbon defects in the twodimensional(2D)mesoporous N-doped carbon nano flakes(NCNF)is a promising technique for improving ORR performance.As a result,the NCNF exhibits more promising ORR activity than Pt/C and similar performance with reported robust catalysts.Comprehensive experimental and theoretical investigations suggest that topologically defected carbon adjacent to the graphitic valley nitrogen is a real active site,rendering optimal energy for the adsorption of ORR intermediates and lowering the total energy barrier for ORR.Also,NCNF-based Zn-air batteries exhibited an excellent power density and specific capacity of~121.10 mW cm^(-2)and~679.86 mA h g_(Zn)^(-1),respectively.This study not only offers new insights into defected carbons with graphitic valley N for ORR but also proposes novel catalyst design principles and provides a solid grasp of the built-in electric field effect on the ORR performance of defective catalysts.展开更多
With the objectives of enhancing the stability,optical properties and visible-light photocatalytic activity of photocatalysts,we modified oxygen vacancy-rich zinc oxide(Vo-ZnO) with graphitic carbon nitride(g-C3N4...With the objectives of enhancing the stability,optical properties and visible-light photocatalytic activity of photocatalysts,we modified oxygen vacancy-rich zinc oxide(Vo-ZnO) with graphitic carbon nitride(g-C3N4). The resulting g-C3N4/Vo-ZnO hybrid photocatalysts showed higher visible-light photocatalytic activity than pure Vo-ZnO and g-C3N4. The hybrid photocatalyst with a g-C3N4 content of 1 wt% exhibited the highest photocatalytic degradation activity under visible-light irradiation(λ≥ 400 nm). In addition,the g-C3N4/Vo-ZnO photocatalyst was not deactivated after five cycles of methyl orange degradation,indicating that it is stable under light irradiation. Finally,a Z-scheme mechanism for the enhanced photocatalytic activity and stability of the g-C3N4/Vo-ZnO hybrid photocatalyst was proposed. The fast charge separation and transport within the g-C3N4/Vo-ZnO hybrid photocatalyst were attributed as the origins of its enhanced photocatalytic performance.展开更多
Sodium-ion batteries(SIBs)are considered one of the most promising energy storage systems for replacing lithium-ion batteries because of the high abundance and low cost of sodium.Iron oxyfluoride(FeOF)is a promising c...Sodium-ion batteries(SIBs)are considered one of the most promising energy storage systems for replacing lithium-ion batteries because of the high abundance and low cost of sodium.Iron oxyfluoride(FeOF)is a promising conversion-based cathode material for SIBs because of its high theoretical capacity of about855 mA h g^(-1),low-cost chemical compositions,and its lower sensitivity to the size of charged carrier ions.However,the poor electrical conductivity and ionic diffusion of FeOF result in a low rate capability and cyclability.In this work,FeOF nanoparticles wrapped by graphitic carbon layers were synthesized using abietic or maleopimaric acid as both the carbon source and organic ligand.In addition,the morphology of the FeOF particles was gradually controlled from rod to spherical shapes,simply depending on the rosin acids.The FeOF nanoparticles prepared with maleopimaric acid showed a large reversible discharge capacity of 356.7 mA h g^(-1)with a fading rate of 0.21%per cycle after 100 cycles at a current density of 100 mA g^(-1)and an excellent rate capability.展开更多
Pure bismuth(Bi) metal-modified graphitic carbon nitride(g-C3N4) composites(Bi-CN) with a pomegranate-like structure were prepared by an in situ method.The Bi-CN composites were used as photocatalysts for the ox...Pure bismuth(Bi) metal-modified graphitic carbon nitride(g-C3N4) composites(Bi-CN) with a pomegranate-like structure were prepared by an in situ method.The Bi-CN composites were used as photocatalysts for the oxidation of nitric oxide(NO) under visible-light irradiation.The inclusion of pure Bi metal in the g-C3N4 layers markedly improved the light absorption of the Bi-CN composites from the ultraviolet to the near-infrared region because of the typical surface plasmon resonance of Bi metal.The separation and transfer of photogenerated charge carriers were greatly accelerated by the presence of built-in Mott-Schottky effects at the interface between Bi metal and g-C3N4.As a result,the Bi-CN composite photocatalysts exhibited considerably enhanced efficiency in the photocatalytic removal of NO compared with that of Bi metal or g-C3N4 alone.The pomegranate-like structure of the Bi-CN composites and an explanation for their improved photocatalytic activity were proposed.This work not only provides a design for highly efficient g-C3N4-based photocatalysts through modification with Bi metal,but also offers new insights into the mechanistic understanding of g-C3N4-based photo catalysis.展开更多
Waste graphitization cathode carbon blocks are a type of hazardous solid waste generated during the aluminum electrolysis process,and their proper disposal is a key step in the resource utilization of discarded graphi...Waste graphitization cathode carbon blocks are a type of hazardous solid waste generated during the aluminum electrolysis process,and their proper disposal is a key step in the resource utilization of discarded graphite.This study utilizes the porous“defect advantage”of a cathode carbon block matrix to prepare silicon-doped and asphalt-coated detoxified and purified waste graphitization cathode carbon blocks for use as high-performance silicon/carbon composite anode materials.The results show that the uniformly silicondoped silicon/carbon composite material features a unique amorphous carbon-encapsulated“locked silicon”structure,which effectively addresses issues such as cathode volume expansion,excessive growth of the solid electrolyte interphase(SEI)film,and poor electrical contact between active materials.Consequently,electrochemical performance is enhanced.After assembly in a half-cell,the PSCC/10%Si@C(purified waste graphitization cathode carbon/10%Si@C)material exhibits optimal electrochemical stability,with an initial charging specific capacity of 514.5 mAh/g at 0.1 C(1 C=170 mA/g)and a capacity retention rate of 95.1%after 100 cycles.At a charge rate of 2.0 C,a specific capacity of 216.9 mAh/g is achieved.This technology provides a new pathway for the economical and high-value utilization of waste cathode carbon blocks and the development of low-cost,high-performance anode materials.展开更多
As one of the most appealing and attractive technologies, photocatalysis is widely used as a promising method to circumvent the environmental and energy problems. Due to its chemical stability and unique physicochemic...As one of the most appealing and attractive technologies, photocatalysis is widely used as a promising method to circumvent the environmental and energy problems. Due to its chemical stability and unique physicochemical, graphitic carbon nitride (g-C3N4) has become research hotspots in the community. However, g-C3N4 photocatalyst still suffers from many problems, resulting in unsatisfactory photocatalytic activity such as low specific surface area, high charge recombination and insufficient visible light utilization. Since 2009, g-C3N4-based heterostructures have attracted the attention of scientists worldwide for their greatly enhanced photocatalytic performance. Overall, this review summarizes the recent advances of g-C3N4-based nanocomposites modified with transition metal sulfide (TMS), including (1) preparation of pristine g-C3N4,(2) modification strategies of g-C3N4,(3) design principles of TMS-modified g-C3N4 heterostructured photocatalysts, and (4) applications in energy conversion. What is more, the characteristics and transfer mechanisms of each classification of the metal sulfide heterojunction system will be critically reviewed, spanning from the following categories:(1) Type I heterojunction,(2) Type II heterojunction,(3) p-n heterojunction,(4) Schottky junction and (5) Z-scheme heterojunction. Apart from that, the application of g-C3N4-based heterostructured photocatalysts in H2 evolution, CO2 reduction, N2 fixation and pollutant degradation will also be systematically presented. Last but not least, this review will conclude with invigorating perspectives, limitations and prospects for further advancing g-C3N4-based heterostructured photocatalysts toward practical benefits for a sustainable future.展开更多
Graphitic carbon nitride(g-C_(3)N_(4))has emerged as a remarkably promising photocatalyst for addressing environmental and energy issues;however,it exhibits only moderate photocatalytic activity because of its low spe...Graphitic carbon nitride(g-C_(3)N_(4))has emerged as a remarkably promising photocatalyst for addressing environmental and energy issues;however,it exhibits only moderate photocatalytic activity because of its low specific surface area and high recombination of carriers.Preparation of crystalline g-C_(3)N_(4) by the molten salt method has proven to be an effective method to improve the photocatalytic activity.However,crystalline g-C_(3)N_(4) prepared by the conventional molten salt method exhibits a less regular morphology.Herein,highly crystalline g-C_(3)N_(4) hollow spheres(CCNHS)were successfully prepared by the molten salt method using cyanuric acid-melamine as a precursor.The higher crystallization of the CCNHS samples not only repaired the structural defects at the surface of the CCNHS samples but also established a built-in electric field between heptazine-based g-C_(3)N_(4) and triazine-based g-C_(3)N_(4).The hollow structure improved the level of light energy utilization and increased the number of active sites for photocatalytic reactions.Because of the above characteristics,the as-prepared CCNHS samples simultaneously realized photocatalytic hydrogen evolution with the degradation of the plasticizer bisphenol A.This research offers a new perspective on the structural optimization of supramolecular self-assembly.展开更多
基金supported by the National Natural Science Foun-dation of China(Grant No.51902041).
文摘Zinc-ion hybrid supercapacitors(ZHSCs)have enormous potential for future applications in electric vehi-cles,portable/wearable electronic gadgets,etc.However,to accelerate ZHSC technology towards market applications,it is necessary to overcome research challenges such as Zn dendrites,low Zn utilization,and all-climate adaptability,as well as to streamline the device assembly process.In this study,we propose a new strategy for the facile construction of ZHSC via two porous carbon fabrics and a Zn plating solution.The cathode and current collector of the device are both porous graphitized carbon fabric(PGCF)pre-pared by high-temperature activation of K2 FeO_(4),and the Li_(2)ZnCl_(4)·9H_(2)O electrolyte is verified to possess excellent Zn plating/stripping efficiency and inhibition of Zn dendrite growth in a Zn-Zn symmetric cell model.As a result,the assembled ZHSC has the maximum energy density of 2.02 mWh cm^(−2)and the highest power density of 11.47 mW cm^(−2),and it can operate for 30,000 cycles without capacity degrada-tion.Furthermore,the destruction of the hydrogen bonding network by the high concentration of Cl−at low temperatures endows it with low freezing point properties and excellent ionic activity at low tem-peratures.The device also operated reliably at-60℃,with a maximum areal capacity of 1.15 mAh cm^(−2).This research offers new findings and insights for the development of high-performance ultra-cryogenic ZHSC devices.
基金supported by National Natural Science Foundation of China(Grant No.51932011,51802356)Innovation-Driven Project of Central South University(No.2020CX024)+3 种基金the Research Support Fund of the Collaborative Innovation Center of Manganese-Zinc-Vanadium Industrial Technology in Hunan Province(No.201809)the Program of Youth Talent Support for Hunan Province(2018RS3098)Hunan Provincial Innovation Foundation for Postgraduate(Grant No.CX2017B045)the Fundamental Research Funds for the Central Universities of Central South University(Grant No.2020zzts075).
文摘Potassium-ion batteries(KIBs)have great potential for applications in large-scale energy storage devices.However,the larger radius of K+leads to sluggish kinetics and inferior cycling performance,severely restricting its practical applicability.Herein,we propose a rational strategy involving a Prussian blue analogue-derived graphitized carbon anode with fast and durable potassium storage capability,which is constructed by encapsulating cobalt nanoparticles in nitrogen-doped graphitized carbon(Co-NC).Both experimental and theoretical results show that N-doping effectively promotes the uniform dispersion of cobalt nanoparticles in the carbon matrix through Co-N bonds.Moreover,the cobalt nanoparticles and strong Co-N bonds synergistically form a threedimensional conductive network,increase the number of adsorption sites,and reduce the diffusion energy barrier,thereby facilitating the adsorption and the diffusion kinetics.These multiple effects lead to enhanced reversible capacities of 305 and 208.6 mAh g^−1 after 100 and 300 cycles at 0.05 and 0.1 A g^−1,respectively,demonstrating the applicability of the Co-NC anode for KIBs.
基金supported by the National Natural Science Foundation of China (21972048, 21802046)the Natural Science Foundation of Guangdong Province (Nos. 2019A1515011138, 2017A030313090, 2017A030310086, 2018A0303130018)。
文摘Cocatalysts play important roles in improving the activity and stability of most photocatalysts.It is of great significance to develop economical,efficient and stable cocatalysts.Herein,using Na2CoFe(CN)6 complex as precursor,a novel noble-metal-free FeCo@NGC cocatalyst(nano-FeCo alloy@N-doped graphitized carbon) is fabricated by a simple pyrolysis method.Coupling with g-C3 N4, the optimal FeCo@NGC/g-C3N4 receives a boosted visible light driven photocatalytic H2 evolution rate of 42.2 μmol h-1, which is even higher than that of 1.0 wt% Pt modified g-C3N4 photocatalyst.Based on the results of density functional theory(DFT) calculations and practical experiment measurements,such outstanding photocatalytic performance of FeCo@NGC/g-C3N4 is mainly attributed to two aspects.One is the accelerated charge transfer behavior,induced by a photogene rated electrons secondary transfer performance on the surface of FeCo alloy nanoparticles.The other is related to the adjustment of H adsorption energy(approaching the standard hydrogen electrode potential) by the presence of external NGC thin layer.Both factors play key roles in the H2 evolution reaction.Such outstanding performance highlights an enormous potential of developing noble-metal-free bimetallic nano-alloy as inexpensive and efficient cocatalysts for solar applications.
基金supported by the National Natural Science Foundation of China (nos. 21771012, 22038001, 51621003)。
文摘Exploring nonprecious electrocatalysts for water splitting with high efficiency and durability is critically important.Herein,bimetallic phosphides are encapsulated into graphitized carbon to construct a C@NiCoP composite nanoarray using bimetallic metal-organic framework(MOF) as a self-sacrificial template.The resulting C@NiCoP exhibits superior performance for pH-universal electrocatalytic hydrogen evolution reaction(HER),particularly representing a low overpotential of 46.3 mV at 10 mA cm^(-2) and Tafel slope of 44.1 mV dec^(-1) in alkaline media.The structural characterizations combined with theoretical calculation demonstrate that tailored electronic structure from bimetal atoms and the synergistic effect with graphitized carbon layer could jointly optimize the adsorption ability of hydrogen on active sites in HER process,and enhance the electrical conductivity as well.In addition,the carbon layer served as a protecting shell also prevents highly dispersed NiCoP components from agglomeration and/or loss in harsh media,finally improving the durability.This work thus provides a new insight into optimizing activity and stability of pH-universal electrocatalysts by the nanostructural design and electronic structure modulation.
基金supported by the National Natural Science Foundation of China (No. 21974045)the Science and Technology Commission of Shanghai Municipality (No. 19142201100)+1 种基金the Fundamental Research Funds for the Central Universities (No. JKJ01211718)the National Key R&D Program of China (No. 2021YFF0701900)。
文摘A novel chromatography stationary phase with a quasi-graphitized carbon modified shell has been developed. Coal pitch was directly carbonized on the surface of porous silica with in-situ carbonization. The carbonized coal pitch coating exhibits some degree of graphitization with a 78 nm-thick layer on the surface of silica and a 0.5 nm-thick layer on the inner surface of the mesopores. Based on the special structure of the graphitized carbon coating, the novel stationary phase can provide multiple interactions such as hydrophobic interaction, π-π interaction and dipole-dipole interaction. The novel composite material exhibited unique separation selectivity and excellent separation efficiency for polar compounds, including imidazoles, nucleosides and pesticides. Besides, the packed column also exhibited great repeatability with the RSDs of the retention time of nucleosides between 0.07%-0.50%(n = 5). Finally, satisfied result was achieved in the separation of fullerenes on the new column, suggesting the great potential in the industrial-scale purification of fullerenes.
基金This work was financially supported by National Key R&D Program of China(2018YFA0507501)the National Natural Science Foundation of China(22074019,21425518,22004017)Shanghai Sailing Program(20YF1405300).
文摘Due to inefficient diagnostic methods,inflammatory bowel disease(IBD)normally progresses into severe complications including cancer.Highly efficient extraction and identification of metabolic fingerprints are of significance for disease surveillance.In this work,we synthesized a layered titania nanosheet doped with graphitized carbon(2D-GC-mTNS)through a simple one-step assembly process for assisting laser desorption ionization mass spectrometry(LDI-MS)for metabolite analysis.Based on the synergistic effect of graphitized carbon and mesoporous titania,2D-GC-mTNS exhibits good extraction ability including high sensitivity(<1 fmolμL−1)and great repeatability toward metabolites.A total of 996 fingerprint spectra were collected from hundreds of native urine samples(including IBD patients and healthy controls),each of which contained 1220 m/z metabolite features.Diagnostic model was further established for precise discrimination of patients from healthy controls,with high area under the curve value of 0.972 and 0.981 toward discovery cohort and validation cohort,respectively.The 2D-GC-mTNS promotes LDI-MS to be close to clinical application,with rapid speed,minimum sample consumption and free of sample pretreatment.
基金supported by the National Natural Science Foundation of China(No.52274346).
文摘Graphitized spent carbon cathode(SCC)is a hazardous solid waste generated in the aluminum electrolysis process.In this study,a flotation-acid leaching process is proposed for the purification of graphitized SCC,and the use of the purified SCC as an anode material for lithium-ion batteries is explored.The flotation and acid leaching processes were separately optimized through one-way experiments.The maximum SCC carbon content(93wt%)was achieved at a 90%proportion of−200-mesh flotation particle size,a slurry concentration of 10wt%,a rotation speed of 1600 r/min,and an inflatable capacity of 0.2 m^(3)/h(referred to as FSCC).In the subsequent acid leaching process,the SCC carbon content reached 99.58wt%at a leaching concentration of 5 mol/L,a leaching time of 100 min,a leaching temperature of 85°C,and an HCl/FSCC volume ratio of 5:1.The purified graphitized SCC(referred to as FSCC-CL)was utilized as an anode material,and it exhibited an initial capacity of 348.2 mAh/g at 0.1 C and a reversible capacity of 347.8 mAh/g after 100 cycles.Moreover,compared with commercial graphite,FSCC-CL exhibited better reversibility and cycle stability.Thus,purified SCC is an important candidate for anode material,and the flotation-acid leaching purification method is suitable for the resourceful recycling of SCC.
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.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.
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supported by the Shanxi Province Central Guidance Fund for Local Science and Technology Development Project(YDZJSX2024D030)the National Natural Science Foundation of China(22075197,22278290)+2 种基金the Shanxi Province Key Research and Development Program Project(2021020660301013)the Shanxi Provincial Natural Science Foundation of China(202103021224079)the Research and Development Project of Key Core and Common Technology of Shanxi Province(20201102018).
文摘The advancement of planar micro-supercapacitors(PMSCs)for micro-electromechanical systems(MEMS)has been significantly hindered by the challenge of achieving high energy and power densities.This study addresses this issue by leveraging screen-printing technology to fabricate high-performance PMSCs using innovative composite ink.The ink,a synergistic blend of few-layer graphene(Gt),carbon black(CB),and NiCo_(2)O_(4),was meticulously mixed to form a conductive and robust coating that enhanced the capacitive performance of the PMSCs.The optimized ink formulation and printing process result in a micro-supercapacitor with an exceptional areal capacitance of 18.95 mF/cm^(2)and an areal energy density of 2.63μW·h/cm^(2)at a current density of 0.05 mA/cm^(2),along with an areal power density of 0.025 mW/cm^(2).The devices demonstrated impressive durability with a capacitance retention rate of 94.7%after a stringent 20000-cycle test,demonstrating their potential for long-term applications.Moreover,the PMSCs displayed excellent mechanical flexibility,with a capacitance decrease of only 3.43%after 5000 bending cycles,highlighting their suitability for flexible electronic devices.The ease of integrating these PMSCs into series and parallel configurations for customized power further underscores their practicality for integrated power supply solutions in various technologies.
基金supported by the Natural Science Foundation of the Jiangsu Higher Education Institutes of China(No.22KJB530006)Hainan Provincial Natural Science Foundation of China(No.824QN267)。
文摘The rapid emergence of drug-resistant bacterial strains undermines the efficacy of conventional antibiotics,necessitating the development of alternative therapies.Antimicrobial photodynamic therapy(PDT)is a promising approach,but its effectiveness is often limited by the suboptimal photocatalytic activity of photosensitizers.In this study,we introduce a novel photoresponsive carbon-based antibacterial agent,Ce6/g-C_(3)N_(4),which combines the photocatalytic properties of graphite-phase carbon nitride(g-C_(3)N_(4))with the photodynamic attributes of chlorin e6(Ce6).This agent,with an average particle size of 250.7 nm,demonstrates significantly enhanced photocatalytic activity.Additionally,the strong affinity of Ce6/g-C_(3)N_(4)for bacteria and efficient delivery of Ce6 result in an inhibition rate exceeding 99%against Gram-positive bacteria and excellent biofilm eradication under light irradiation.In vivo experiments reveal that Ce6/gC_(3)N_(4)effectively inhibits bacterial growth on wounds,and promotes wound healing post-light treatment,while maintaining good biocompatibility.Overall,the Ce6/g-C_(3)N_(4)antibacterial agent synergizes photodynamic and photocatalytic mechanisms,offering a new avenue for the photo-mediated,multi-strategic treatment of bacterial infections and wound healing.
基金supported by the National Natural Science Foundation of China(No.52173267)the Key Laboratory of High Temperature Electromagnetic Materials and Structure of MOE(No.KB202402).
文摘Graphitic carbon nitride(g-C_(3)N_(4))has garnered significant attention due to its remarkable advantages such as lightweight,exceptional chemical stability and defect-rich surface.Nevertheless,its inadequate electrical conductivity and impedance matching hindered the practical implementation in the electromagnetic wave absorption(EMWA)field.To address these challenges,we developed a composites system of carbon spheres/g-C_(3)N_(4)(CCN)through a supramolecular self-assembly strategy,subsequently integrated with reduced graphene oxide(RGO)via a water bath method.Systematic investigation revealed that the EMWA performance of CCN/RGO composites exhibited a distinct dependence(a trend of first increasing and then decreasing)on RGO content.Especially,when the mass ratio of RGO to CCN was 20%,the CCN/RGO composite brought a minimum reflection loss value of-45.40 dB at 13.44 GHz and a broad effective absorbing bandwidth of 6.32 GHz at 2.19 mm.First-principles calculations based on density functional theory suggested that the constructed heterostructure effectively facilitated electron mobility and charge redistribution,boosting both conductive loss and polarization loss mechanisms.The exceptional absorption performance was ascribed to the synergistic effects of conductive loss,relaxation loss,and suitable impedance matching.As a results,this work provided a rational design strategy for high-performance g-C_(3)N_(4)-based EMWA materials.
基金supported by the National Natural Science Foundation of China(22262010,22062005,22165005,U20A20128)Guangxi Science and Technology Fund for Distinguished HighTalent Introduction Program(AC22035091)Guangxi Science Fund for Distinguished Young Scholars(2019GXNSFFA245016)。
文摘Rational design of defected carbons adjacent to nitrogen(N)dopants is a fascinating but challenging approach for enhancing the catalytic performance of N-doped carbon.Meanwhile,the combined effect of heteroatom doping and defect engineering can efficiently increase the oxygen reduction reaction(ORR)ability of inactive carbons through charge redistribution.Herein,we report that an enhanced built-in electric field caused by the combined effect of N-doping and carbon defects in the twodimensional(2D)mesoporous N-doped carbon nano flakes(NCNF)is a promising technique for improving ORR performance.As a result,the NCNF exhibits more promising ORR activity than Pt/C and similar performance with reported robust catalysts.Comprehensive experimental and theoretical investigations suggest that topologically defected carbon adjacent to the graphitic valley nitrogen is a real active site,rendering optimal energy for the adsorption of ORR intermediates and lowering the total energy barrier for ORR.Also,NCNF-based Zn-air batteries exhibited an excellent power density and specific capacity of~121.10 mW cm^(-2)and~679.86 mA h g_(Zn)^(-1),respectively.This study not only offers new insights into defected carbons with graphitic valley N for ORR but also proposes novel catalyst design principles and provides a solid grasp of the built-in electric field effect on the ORR performance of defective catalysts.
基金supported by the National Basic Research Program of China(2011CB933700)the National Natural Science Foundation of China(21271165)~~
文摘With the objectives of enhancing the stability,optical properties and visible-light photocatalytic activity of photocatalysts,we modified oxygen vacancy-rich zinc oxide(Vo-ZnO) with graphitic carbon nitride(g-C3N4). The resulting g-C3N4/Vo-ZnO hybrid photocatalysts showed higher visible-light photocatalytic activity than pure Vo-ZnO and g-C3N4. The hybrid photocatalyst with a g-C3N4 content of 1 wt% exhibited the highest photocatalytic degradation activity under visible-light irradiation(λ≥ 400 nm). In addition,the g-C3N4/Vo-ZnO photocatalyst was not deactivated after five cycles of methyl orange degradation,indicating that it is stable under light irradiation. Finally,a Z-scheme mechanism for the enhanced photocatalytic activity and stability of the g-C3N4/Vo-ZnO hybrid photocatalyst was proposed. The fast charge separation and transport within the g-C3N4/Vo-ZnO hybrid photocatalyst were attributed as the origins of its enhanced photocatalytic performance.
基金supported by the Dong-A University research fund。
文摘Sodium-ion batteries(SIBs)are considered one of the most promising energy storage systems for replacing lithium-ion batteries because of the high abundance and low cost of sodium.Iron oxyfluoride(FeOF)is a promising conversion-based cathode material for SIBs because of its high theoretical capacity of about855 mA h g^(-1),low-cost chemical compositions,and its lower sensitivity to the size of charged carrier ions.However,the poor electrical conductivity and ionic diffusion of FeOF result in a low rate capability and cyclability.In this work,FeOF nanoparticles wrapped by graphitic carbon layers were synthesized using abietic or maleopimaric acid as both the carbon source and organic ligand.In addition,the morphology of the FeOF particles was gradually controlled from rod to spherical shapes,simply depending on the rosin acids.The FeOF nanoparticles prepared with maleopimaric acid showed a large reversible discharge capacity of 356.7 mA h g^(-1)with a fading rate of 0.21%per cycle after 100 cycles at a current density of 100 mA g^(-1)and an excellent rate capability.
基金supported by the National Program on Key Basic Research Project (2016YFA0203000)the Early Career Scheme (ECS 809813) from the Research Grant Council, Hong Kong SAR Government+2 种基金the Croucher Foundation Visitorship for PRC Scholars 2015/16 at The Education University of Hong Kongthe National Natural Science Foundation of China (51672312, 21373275)the Program for New Century Excellent Talents in University (NCET-12-0668)~~
文摘Pure bismuth(Bi) metal-modified graphitic carbon nitride(g-C3N4) composites(Bi-CN) with a pomegranate-like structure were prepared by an in situ method.The Bi-CN composites were used as photocatalysts for the oxidation of nitric oxide(NO) under visible-light irradiation.The inclusion of pure Bi metal in the g-C3N4 layers markedly improved the light absorption of the Bi-CN composites from the ultraviolet to the near-infrared region because of the typical surface plasmon resonance of Bi metal.The separation and transfer of photogenerated charge carriers were greatly accelerated by the presence of built-in Mott-Schottky effects at the interface between Bi metal and g-C3N4.As a result,the Bi-CN composite photocatalysts exhibited considerably enhanced efficiency in the photocatalytic removal of NO compared with that of Bi metal or g-C3N4 alone.The pomegranate-like structure of the Bi-CN composites and an explanation for their improved photocatalytic activity were proposed.This work not only provides a design for highly efficient g-C3N4-based photocatalysts through modification with Bi metal,but also offers new insights into the mechanistic understanding of g-C3N4-based photo catalysis.
基金supported by the National Natural Science Foundation of China(No.52274346).
文摘Waste graphitization cathode carbon blocks are a type of hazardous solid waste generated during the aluminum electrolysis process,and their proper disposal is a key step in the resource utilization of discarded graphite.This study utilizes the porous“defect advantage”of a cathode carbon block matrix to prepare silicon-doped and asphalt-coated detoxified and purified waste graphitization cathode carbon blocks for use as high-performance silicon/carbon composite anode materials.The results show that the uniformly silicondoped silicon/carbon composite material features a unique amorphous carbon-encapsulated“locked silicon”structure,which effectively addresses issues such as cathode volume expansion,excessive growth of the solid electrolyte interphase(SEI)film,and poor electrical contact between active materials.Consequently,electrochemical performance is enhanced.After assembly in a half-cell,the PSCC/10%Si@C(purified waste graphitization cathode carbon/10%Si@C)material exhibits optimal electrochemical stability,with an initial charging specific capacity of 514.5 mAh/g at 0.1 C(1 C=170 mA/g)and a capacity retention rate of 95.1%after 100 cycles.At a charge rate of 2.0 C,a specific capacity of 216.9 mAh/g is achieved.This technology provides a new pathway for the economical and high-value utilization of waste cathode carbon blocks and the development of low-cost,high-performance anode materials.
基金supported by Xiamen University Malaysia Research Fund (XMUMRF/2019-C3/IENG/0013)financial assistance and faculty start-up grants/supports from Xiamen University~~
文摘As one of the most appealing and attractive technologies, photocatalysis is widely used as a promising method to circumvent the environmental and energy problems. Due to its chemical stability and unique physicochemical, graphitic carbon nitride (g-C3N4) has become research hotspots in the community. However, g-C3N4 photocatalyst still suffers from many problems, resulting in unsatisfactory photocatalytic activity such as low specific surface area, high charge recombination and insufficient visible light utilization. Since 2009, g-C3N4-based heterostructures have attracted the attention of scientists worldwide for their greatly enhanced photocatalytic performance. Overall, this review summarizes the recent advances of g-C3N4-based nanocomposites modified with transition metal sulfide (TMS), including (1) preparation of pristine g-C3N4,(2) modification strategies of g-C3N4,(3) design principles of TMS-modified g-C3N4 heterostructured photocatalysts, and (4) applications in energy conversion. What is more, the characteristics and transfer mechanisms of each classification of the metal sulfide heterojunction system will be critically reviewed, spanning from the following categories:(1) Type I heterojunction,(2) Type II heterojunction,(3) p-n heterojunction,(4) Schottky junction and (5) Z-scheme heterojunction. Apart from that, the application of g-C3N4-based heterostructured photocatalysts in H2 evolution, CO2 reduction, N2 fixation and pollutant degradation will also be systematically presented. Last but not least, this review will conclude with invigorating perspectives, limitations and prospects for further advancing g-C3N4-based heterostructured photocatalysts toward practical benefits for a sustainable future.
文摘Graphitic carbon nitride(g-C_(3)N_(4))has emerged as a remarkably promising photocatalyst for addressing environmental and energy issues;however,it exhibits only moderate photocatalytic activity because of its low specific surface area and high recombination of carriers.Preparation of crystalline g-C_(3)N_(4) by the molten salt method has proven to be an effective method to improve the photocatalytic activity.However,crystalline g-C_(3)N_(4) prepared by the conventional molten salt method exhibits a less regular morphology.Herein,highly crystalline g-C_(3)N_(4) hollow spheres(CCNHS)were successfully prepared by the molten salt method using cyanuric acid-melamine as a precursor.The higher crystallization of the CCNHS samples not only repaired the structural defects at the surface of the CCNHS samples but also established a built-in electric field between heptazine-based g-C_(3)N_(4) and triazine-based g-C_(3)N_(4).The hollow structure improved the level of light energy utilization and increased the number of active sites for photocatalytic reactions.Because of the above characteristics,the as-prepared CCNHS samples simultaneously realized photocatalytic hydrogen evolution with the degradation of the plasticizer bisphenol A.This research offers a new perspective on the structural optimization of supramolecular self-assembly.