Electrocatalytic nitrate reduction reaction(NO3RR)represents a sustainable and environmentally benign route for ammonia(NH3)synthesis.However,NO3RR is still limited by the competition from hydrogen evolution reaction(...Electrocatalytic nitrate reduction reaction(NO3RR)represents a sustainable and environmentally benign route for ammonia(NH3)synthesis.However,NO3RR is still limited by the competition from hydrogen evolution reaction(HER)and the high energy barrier in the hydrogenation step of nitrogen-containing intermediates.Here,we report a selective etching strategy to construct Ru M nanoalloys(M=Fe,Co,Ni,Cu)uniformly dispersed on porous nitrogen-doped carbon substrates for efficient neutral NH3electrosynthesis.Density functional theory calculations confirm that the synergic effect between Ru and transition metal M modulates the electronic structure of the alloy,significantly lowering the energy barrier for the conversion of*NO_(2)to*HNO_(2).Experimentally,the optimized Ru Fe-NC catalyst achieves 100%Faraday efficiency with a high yield rate of 0.83 mg h^(-1)mg^(-1)catat a low potential of-0.1 V vs.RHE,outperforming most reported catalysts.In situ spectroscopic analyses further demonstrate that the Ru M-NC effectively promotes the hydrogenation of nitrogen intermediates while inhibiting the formation of hydrogen radicals,thereby reducing HER competition.The Ru FeNC assembled Zn-NO_(3)^(-)battery achieved a high open-circuit voltage and an outstanding power density and capacity,which drive selective NO_(3)^(-)conversion to NH3.This work provides a powerful synergistic design strategy for efficient NH3electrosynthesis and a general framework for the development of advanced multi-component catalysts for sustainable nitrogen conversion.展开更多
Zinc telluride(ZnTe)with high density and low cost is considered as promising anode for sodium-ion batteries.However,ZnTe suffers from continuous capacity degradation owing to the low electronic conductivity,large vol...Zinc telluride(ZnTe)with high density and low cost is considered as promising anode for sodium-ion batteries.However,ZnTe suffers from continuous capacity degradation owing to the low electronic conductivity,large volume expansion,and high ion-diffusion energy barriers.Herein,the nitrogen-doped carbon confined ZnTe polyhedron heterostructure(ZnTe/NC)is proposed,exploiting its orbital rehybridization and the realignment of energy level to improve storage performance.Systematic ex situ/in situ characterizations and simulations demonstrated that the elaborate ZnTe/NC offers abundant electron/ion transport pathways,accelerates Na^(+)diffusion kinetics,and alleviates huge volume expansion.Notably,the nitrogen-doped carbon-support interaction induced via electron transfer between ZnTe sites and support elevates the energy level of Zn 3d orbital,greatly enhancing ion adsorption capability and reducing the ion diffusion barrier.As a result,the ZnTe/NC anode delivers a high discharge capacity of 470.5 mAh g^(−1)and long cycling durability over 1000 cycles.This work uncovers that optimizing sodium ion adsorption and diffusion via d-orbital energy level modulation enabled by nitrogen-doped support interaction is an effective method for developing high-performance transition metal telluride anodes for alkali ion storage.展开更多
Nitrogen doping is a promising way to modulate the electrical properties of graphene to realize graphene-based electronics and promise fascinating properties and applications.Herein,we report a method to noncovalently...Nitrogen doping is a promising way to modulate the electrical properties of graphene to realize graphene-based electronics and promise fascinating properties and applications.Herein,we report a method to noncovalently assembly titanium(Ⅳ) bis(ammoniumlactato) dihydroxide(Ti complex) on nitrogen-doped graphene to create a reliable hybrids which can be used as a reversible chemical induced switching.As the adsorption and desorption of Ti complex in sequential treatments,the conductance of the nitrogen-doped graphene transistors was finely modulated.Control experiments with pristine graphene clearly demonstrated the important effort of the nitrogen in this chemical sensor.Under optimized conditions,nitrogen-doped graphene transistors open up new ways to develop multifunctional devices with high sensitivity.展开更多
Phosphate residue is regarded as a hazardous waste, which could potentially create significant environmental and health problems if it is not properly treated and disposed of. In this study, nitrogen-doped carbon nano...Phosphate residue is regarded as a hazardous waste, which could potentially create significant environmental and health problems if it is not properly treated and disposed of. In this study, nitrogen-doped carbon nanotubes-FePO_4(NCNTs-FePO_4) composite was successfully synthesized from phosphate residue, and its application as an effective catalyst was explored. Firstly, an effective method was developed to recover FePO_4 from phosphate residue, achieving an impressive FePO_4 mass recovery rate of 98.14%. Then, the NCNTsFePO_4 catalyst was synthesized from the recovered FePO_4 by two main reactions, including surface modification and chemical vapor deposition. Finally, the synthesized NCNTs-FePO_4 was applied to photo-degrade 15 mg/L Rhodamine B(RhB) in a Fenton-like system. The results showed that 98.9% of RhB could be degraded in 60 min, closely following the pseudofirst-order kinetics model. It was found that even after six consecutive cycles, NCNTs-FePO_4 still retained a high catalytic capacity(>50%). Moreover, ·OH radicals participating in the RhB degradation process were evidenced using quenching experiments and electron paramagnetic resonance analysis, and a rational mechanism was proposed. It was demonstrated that the materials synthesized from hazardous phosphate residue can be used as an effective catalyst for dye removal.展开更多
Aniline,pyrrole and phenanthroline,which have different nitrogen compositions,are used as carbon precursors to synthesize nitrogen-doped ordered mesoporous carbons（NOMCs） by the nanocasting method.The effect of the ...Aniline,pyrrole and phenanthroline,which have different nitrogen compositions,are used as carbon precursors to synthesize nitrogen-doped ordered mesoporous carbons（NOMCs） by the nanocasting method.The effect of the precursor on the resultant NOMC is extensively investigated by nitrogen adsorption-desorption measurements,scanning electron microscopy,X-ray photoelectron spectroscopy（XPS）,cyclic voltammetry and rotating ring-disk electrode measurements.Salient findings are as follows.First,the precursor has a significant influence on the specific surface area and textural properties.The NOMC materials derived from pyrrole（C-PY-900：765 m^2/） and phenanthroline（C-Phen-900：746 m^2/） exhibit higher specific surface areas than the aniline analog（C-PA-900：569 m^2/）.Second,the XPS results indicate that the total nitrogen content（ca.3.1–3.3 at%） is similar for the three carbon sources,except for a slight difference in the nitrogen configuration.Furthermore,the content of the nitrogen-activated carbon atoms is found to closely depend on the precursor,which is the highest for the phenanthroline-derived carbon.Third,the electrochemical results reveal that the electrocatalytic activity follows in the order C-PA-900 C-PY-900 C-Phen-900,confirming that the nitrogen-activated carbon atoms are the active sites for the oxygen reduction reaction（ORR）.In summary,the precursor has considerable influence on the composition and textural properties of the NOMC materials,of which the ORR electrocatalytic activity can be enhanced through optimization of the NOMCs.展开更多
Traditionally reduced graphene oxide(RGO)-based electromagnetic wave(EMW)absorbing materials have poor absorption effectiveness due to impedance mismatch caused by skin effect.The introduction of structural defects an...Traditionally reduced graphene oxide(RGO)-based electromagnetic wave(EMW)absorbing materials have poor absorption effectiveness due to impedance mismatch caused by skin effect.The introduction of structural defects and the design of heterogeneous interfaces play a crucial role in enhancing the polarization effect of EMW absorbers.In this study,nitrogen-doped reduced graphene oxide/zinc ferrite@nitrogen-doped carbon(NRGO/ZnFe_(2)O_(4)@NC)ternary composite with rich heterogeneous interfaces is constructed by combining solvothermal reaction,in-situ polymerization,annealing treatment with subsequent hydrothermal reaction.The research results have shown that the obtained NRGO/ZnFe_(2)O_(4)@NC ternary composite exhibits a unique core-shell structure and excellent EMW absorption performance.At a thickness of 2.61 mm,the maximum effective absorption bandwidth can reach 7.2 GHz,spanning the entire Ku-band and a portion of the X-band,and the minimum reflection loss is-61.1 dB,which is superior to most reported RGO-based EMW absorbers.The excellent EMW absorbing ability is mainly ascribed to the optimized impedance matching and the enhanced polarization loss caused by the abundant heterogeneous interfaces and structural defects derived from heteroatomic nitrogen doping.Furthermore,the radar cross section in the far field is simulated by a computer simulation technique.This study provides a novel way to prepare core-shell magnetic carbon composites as highly efficient and broadband EMW absorbers.展开更多
Nitrogen-doped carbon nanotubes （NCNTs） were used as a support for iron （Fe） nanoparticles applied in car- bon dioxide （CO_2） hydrogenation at 633 K and 25 bar （1 bar = 10-5 Pa）. The Fe/NCNT catalyst promoted ...Nitrogen-doped carbon nanotubes （NCNTs） were used as a support for iron （Fe） nanoparticles applied in car- bon dioxide （CO_2） hydrogenation at 633 K and 25 bar （1 bar = 10-5 Pa）. The Fe/NCNT catalyst promoted with both potassium （K） and manganese （Mn） showed high performance in CO_2 hydrogenation, reaching 34.9% conversion with a gas hourly space velocity （GHSV） of 3.1 L-（g·h）-1. Product selectivities were high for olefin products and low for short-chain alkanes for the K-promoted catalysts. When Fe/NCNT catalyst was promot- ed with both K and Mn, the catalytic activity was stable for 60 h of reaction time. The structural effect of the Mn promoter was demonstrated by X-ray diffraction （XRD）, temperature-programmed reduction （TPR） with molecular hydrogen （H2）, and in situ X-ray absorption near-edge structure （XANES） analysis. The Mn pro- moter stabilized wtistite （FeO） as an intermediate and lowered the TPR onset temperature. Catalytic ammo- nia （NH_3） decomposition was used as an additional probe reaction for characterizing the promoter effects. The Fe/NCNT catalyst promoted with both K and Mn had the highest catalytic activity, and the Mn-promoted Fe/NCNT catalysts had the highest thermal stability under reducing conditions.展开更多
Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NH...Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NHMC/Ni/NiO)nanocomposite for developing high-capacity LIBs anode materials through carbonization and selective etching strategies.The synthesized NMHC/Ni/NiO-0.33 composite exhibited a highly regular microstructure with well-dispersed Ni/NiO particles.The composite had a surface area of 408 m^(2)·g^(−1),a mesopore ratio of 75.0%,and a pyridine–nitrogen ratio of 58.9%.The introduction of nitrogen atoms reduced the disordered structure of lignin mesoporous carbon and enhanced its electrical conductivity,thus improving the lithium storage capabilities of the composite.Following 100 cycles at a current density of 0.2 A·g^(−1),the composite demonstrated enhanced Coulomb efficiency and rate performance,achieving a specific discharge capacity of 1230.9 mAh·g^(−1).At a high-current density of 1 A·g^(−1),the composite exhibited an excellent specific discharge capacity of 714.6 mAh·g^(−1).This study presents an innovative method for synthesizing high-performance anode materials of LIBs.展开更多
In this report, nitrogen-doped porous carbons were synthesized from polyacrylonitrile fiber by a facile two-step synthesis process i.e. carbonization followed by KOH activation. Activation temperature and KOH/carbon r...In this report, nitrogen-doped porous carbons were synthesized from polyacrylonitrile fiber by a facile two-step synthesis process i.e. carbonization followed by KOH activation. Activation temperature and KOH/carbon ratio are two parameters to tune the porosity and surface chemical properties of sorbents. The as-obtained sorbents were carefully characterized.Special attention was paid concerning the change of sorbents’ morphology with respect to synthesis conditions. Under the activation temperatures of this study, the sorbents can still retain their fibrous structure when the KOH/carbon mass ratio is 1. Further increasing the KOH amount will destroy the original morphology of polyacrylonitrile fiber. CO_(2)adsorption performance tests show that a sorbent retaining the fibrous shape possesses the highest CO_(2)uptake of 3.95 mmol/g at 25℃and 1 bar. Comprehensive investigation found that the mutual effect of narrow microporosity and doped N content govern the CO_(2)adsorption capacity of these adsorbents. Furthermore, these polyacrylonitrile fiber-derived carbons present multiple outstanding CO_(2)capture properties such as excellent recyclability, high CO_(2)/N_(2)selectivity, fast adsorption kinetics, suitable heat of adsorption, and good dynamic adsorption capacity. Hence, nitrogen-doped porous carbons with fibrous structure are promising in CO_(2)capture.展开更多
Among the synthesis techniques for graphene,chemical vapor deposition(CVD)enables the direct growth of graphene films on insulating substrates.Its advantages include uniform coverage,high quality,scalability,and compa...Among the synthesis techniques for graphene,chemical vapor deposition(CVD)enables the direct growth of graphene films on insulating substrates.Its advantages include uniform coverage,high quality,scalability,and compatibility with industrial processes.Graphene is chemically inert and has a zero-bandgap which poses a problem for its use as a functional layer,and nitrogen doping has become an important way to overcome this.Post-plasma treatment has been explored for the synthesis of nitrogen-doped graphene,but the procedures are intricate and not suitable for large-scale production.We report the direct synthesis of nitrogen-doped graphene on a 4-inch sapphire wafer by ethanol-assisted CVD employing pyridine as the carbon feedstock,where the nitrogen comes from the pyridine and the hydroxyl group in ethanol improves the quality of the graphene produced.Additionally,the types of nitrogen dopant produced and their effects on III-nitride epitaxy were also investigated,resulting in the successful illumination of LED devices.This work presents an effective synthesis strategy for the preparation of nitrogen-doped graphene,and provides a foundation for designing graphene functional layers in optoelectronic devices.展开更多
The most energy-inefficient step in the oxygen evolution reaction(OER), which involves a complicated four-electron transfer process, limits the efficiency of the electrochemical water splitting. Here, well-defined Ni/...The most energy-inefficient step in the oxygen evolution reaction(OER), which involves a complicated four-electron transfer process, limits the efficiency of the electrochemical water splitting. Here, well-defined Ni/Co3O4 nanoparticles coupled with N-doped carbon hybrids(Ni/Co3O4@NC) were synthesized via a facile impregnation-calcination method as efficient electrocatalysts for OER in alkaline media. Notably, the impregnation of the polymer with Ni and Co ions in the first step ensured the homogeneous distribution of metals, thus guaranteeing the subsequent in situ calcination reaction, which produced well-dispersed Ni and Co3O4 nanoparticles. Moreover, the N-doped carbon matrix formed at high temperatures could effectively prevent the aggregation and coalescence, and regulate the electronic configuration of active species. Benefiting from the synergistic effect between the Ni, Co3O4, and NC species, the obtained Ni/Co3O4@NC hybrids exhibited enhanced OER activities and remarkable stability in an alkaline solution with a smaller overpotential of 350 m V to afford 10 m A cm-2, lower Tafel slope of 52.27 m V dec-1, smaller charge-transfer resistance, and higher double-layer capacitance of 25.53 m F cm-2 compared to those of unary Co3O4@NC or Ni@NC metal hybrids. Therefore, this paper presents a facile strategy for designing other heteroatom-doped oxides coupled with ideal carbon materials as electrocatalysts for the OER.展开更多
Non-noble metal electrocatalysis has witnessed rapid and profound performance improvements owing to the emergence of advanced nanosynthetic techniques.Integration of these nanotechniques can lead to synergistic perfor...Non-noble metal electrocatalysis has witnessed rapid and profound performance improvements owing to the emergence of advanced nanosynthetic techniques.Integration of these nanotechniques can lead to synergistic performance enhancement,but such system-engineering strategies are difficult to achieve because of the lack of effective synthesis method.We hereby demonstrate an integrated approach that combines most of the existing nanotechniques in a facile one-pot synthesis.Material characterization reveals that the product shows key features intended by techniques including morphological,structural,doping,heterointerface,and surface wetting engineering.The as-obtained nitrogen-doped hierarchical heterostructured MoS_(x)/Ni_(3)S_(2)nanowires show an overpotential that is only50 mV higher than commercial Pt/C for hydrogen evolution reaction over current densities from 10 to 150 mA cm^(-2).Correlations between the adopted nanotechniques and the electrochemical reaction rates are established by evaluating the impacts of individual techniques on the activation energy,pre-exponential factor,and transfer coefficient.This indepth analysis provides a full account of the synergistic effects and the overall improvement in electrocatalytic performance of hydrogen evolution reaction.This work manifests a generic strategy for multipurpose material design in non-noble metal electrocatalysis.展开更多
We synthesized CN11,a carbon nitride material rich in sp^(3)hybrid graphitic nitrogen(sp^(3)-N),employing a facile oxalic acid-assisted melamine molecular assembly strategy.CN11 promoted the formation of Pd nanopartic...We synthesized CN11,a carbon nitride material rich in sp^(3)hybrid graphitic nitrogen(sp^(3)-N),employing a facile oxalic acid-assisted melamine molecular assembly strategy.CN11 promoted the formation of Pd nanoparticles(NPs)predominantly exposing{200}facets,termed Pd/CN11-2.This facet-specific configuration significantly boosted hydrogen adsorption,leading to notable improvements in catalytic activity.Compared to Pd/XC-72-2 and Pd/g-C_(3)N_(4)-2,Pd/CN11-2 exhibited a remarkable two-fold and nineteen-fold increase in catalytic yield for hydrazo compound hydrogenation,respectively.Pd/CN11-2 also demonstrated robust performance across a range of reaction conditions,maintaining excellent yield.This study emphasizes the critical role of tailored support structures in controlling Pd NPs facets,thereby enhancing hydrogenation efficiency.It provides valuable insights for advancing the industrial application of Pd-based catalysts,underscoring the importance of strategic support modulation for optimizing catalytic performance.展开更多
Development of efficient and stable metal catalysts for the selective aqueous phase hydrodeoxygenation(HDO)of biomass-derived oxygenates to value-added biofuels is highly desired.An innovative surface microenvironment...Development of efficient and stable metal catalysts for the selective aqueous phase hydrodeoxygenation(HDO)of biomass-derived oxygenates to value-added biofuels is highly desired.An innovative surface microenvironment modulation strategy was used to construct the nitrogen-doped hollow carbon sphere encapsulated with Pd(Pd@NHCS-X,X:600–800)nanoreactors for catalytic HDO of biomass-derived vanillin in water.The specific surface microenvironments of Pd@NHCS catalysts including the electronic property of active Pd centers and the surface wettability and porous structure of NHCS supports could be well-controlled by the calcination temperature of catalysts.Intrinsic kinetic evaluations demonstrated that the Pd@NHCS-600 catalyst presented a high turnover frequency of 337.77 h^(–1)and a low apparent activation energy of 18.63 kJ/mol.The excellent catalytic HDO performance was attributed to the unique surface microenvironment of Pd@NHCS catalyst based on structure-performance relationship analysis and DFT calculations.It revealed that pyridinic N species dominated the electronic property regulation of Pd sites through electronic metal-support interaction(EMSI)and produced numerous electron-rich active Pd centers,which not only intensified the dissociation and activation of H2 molecules,but also substantially improved the activation capability of vanillin via the enhanced adsorption of–C=O group.The fine hydrophilicity and abundant porous structure promoted the uniform dispersion of catalyst and ensured the effective access of reactants to catalytic active centers in water.Additionally,the Pd@NHCS-600 catalyst exhibited excellent catalytic stability and broad substrate applicability for the selective aqueous phase HDO of various biomass-derived carbonyl compounds.The proposed surface microenvironment modulation strategy will provide a new consideration for the rational design of high-performance nitrogen-doped carbon-supported metal catalysts for catalytic biomass transformation.展开更多
Utilizing nitrate(NO_(3)^(-))as the nitrogen source to produce ammonia can effectively remove NO_(3)^(-)pollutant while obtaining valuable ammonia,and the understanding of the mechanisms is essential for the design of...Utilizing nitrate(NO_(3)^(-))as the nitrogen source to produce ammonia can effectively remove NO_(3)^(-)pollutant while obtaining valuable ammonia,and the understanding of the mechanisms is essential for the design of new catalysts.In this work,by using density functional theory calculations,the electroreduction mechanisms of nitrate reduction reaction(NO_(3)RR)on transition metal single atom supported on 3N-coordinated N-doped graphene(TM/N_(3)-G)are systematically investigated.It is found that the protonation of ^(*)OH acts as the potential determing steps except for the traditionally considered ^(*)NO_(3)/^(*)NO/^(*)NO_(2) protonation step and the desorption of water may play an important role for NO_(3)RR on some TM/N_(3)-G.By considering the stability of single-atom catalyst(SAC),the preferential adsorption of NO_(3)^(-)larger than H and H_(2)O,the limiting potential of whole NO_(3)RR,the selectivity toward NH3,V(Mn,Os)/pyrrolic-N_(3)-G and Mn(Ru,Ir)/pyridinic-N_(3)-G are screened out as potential SACs for NO_(3)RR.This work provides an understanding of the NO_(3)RR mechanism and highlights several promising NO_(3)RR catalysts based on the TM/N_(3)-G system.展开更多
Zn-air battery(ZAB)has garnered significant attention owing to its environmental friendliness and safety attributes.A critical challenge in advancing ZAB technology lies in the development of high-performance and cost...Zn-air battery(ZAB)has garnered significant attention owing to its environmental friendliness and safety attributes.A critical challenge in advancing ZAB technology lies in the development of high-performance and cost-effective electrocatalysts for oxygen redox reactions(OER and ORR).Herein,we report Co/Fe carbon-supported composites as efficient bifunctional catalyst encapsulated in oxidative ammonolysis modified lignin-derived N-doped biochar(Co Fe-Co_(x)N@NOALC).It exhibited exceptional electrochemical performance in aqueous ZAB owing to their uniform dispersed and small particle size,with a peak power density of 154 mW/cm^(2)and a specific capacity of 770 mAh/g.Most notably,it exhibited a long cycle stability,surpassing 1500 h at a current density of 10 mA/cm^(2),with a mere 11.4%decrease in the chargedischarge efficiency of the battery.This study proposes a viable strategy for enhancing the performance and reducing the cost of Zn-air batteries through the utilization of biomass-derived materials.展开更多
Solar-induced water oxidation reaction(WOR)for oxygen evolution is a critical step in the transformation of Earth's atmosphere from a reducing to an oxidation one during its primordial stages.WOR is also associate...Solar-induced water oxidation reaction(WOR)for oxygen evolution is a critical step in the transformation of Earth's atmosphere from a reducing to an oxidation one during its primordial stages.WOR is also associated with important reduction reactions,such as oxygen reduction reaction(ORR),which leads to the production of hydrogen peroxide(H_(2)O_(2)).These transitions are instrumental in the emergence and evolution of life.In this study,transition metals were loaded onto nitrogen-doped carbon(NDC)prepared under the primitive Earth's atmospheric conditions.These metal-loaded NDC samples were found to catalyze both WOR and ORR under light illumination.The chemical pathways initiated by the pristine and metal-loaded NDC were investigated.This study provides valuable insights into potential mechanisms relevant to the early evolution of our planet.展开更多
Nitrogen-doped diamond-like carbon （DLC：N） films prepared by the filtered cathodic vacuum arc technology are functionalized with various chemical molecules including dopamine （DA）, 3-Aminobenzeneboronic acid （A...Nitrogen-doped diamond-like carbon （DLC：N） films prepared by the filtered cathodic vacuum arc technology are functionalized with various chemical molecules including dopamine （DA）, 3-Aminobenzeneboronic acid （APBA）, and adenosine triphosphate （ATP）, and the impacts of surface functionalities on the surface morphologies, compositions, microstructures, and cell compatibility of the DLC：N films are systematically investigated. We demonstrate that the surface groups of DLC：N have a significant effect on the surface and structural properties of the film. The activity of PC12 cells depends on the particular type of surface functional groups of DLC：N films regardless of surface roughness and wettability. Our research offers a novel way for designing functionalized carbon films as tailorable substrates for biosensors and biomedical engineering applications.展开更多
The recycling of plastics is a significant global concern.Due to the thermosetting properties of melamineformaldehyde(MF)resin plastics,which make heating and melting difficult,their recycling and reuse pose substanti...The recycling of plastics is a significant global concern.Due to the thermosetting properties of melamineformaldehyde(MF)resin plastics,which make heating and melting difficult,their recycling and reuse pose substantial challenges.In this study,we developed nitrogen-doped(N-doped)carbon materials through scalable carbonization of MF resin plastic waste.This metal-free N-doped carbon catalyst achieved a hydrogen peroxide(H_(2)O_(2))production rate of 971.6 mmol gcatalyst^(-1)h^(-1)with a Faradaic efficiency for H_(2)O_(2)(FEH_(2)O_(2))exceeding 90%under acidic conditions.Additionally,a flow cell utilizing this carbon catalyst demonstrated a production rate of 11.3 mol cm^(-2)h^(-1)(22.5 mol g_(catalyst)^(-1)h^(-1))and maintained a record-high current density of approximately 530 mA cm^(-2)over 300 h.In-situ electrochemical surface-enhanced Raman spectroscopy and density functional theory calculations revealed the presence of porphyrin-like carbon defects,which serve as active sites for the continuous and stable generation of^(*)OOH species.The nitrogen-doped carbon materials obtained from large-scale carbonization of MF plastic waste exhibit abundant active sites,making them highly promising electrocatalysts for the two-electron oxygen reduction reaction(2e^(-)ORR).展开更多
The in-flight heating process of cerium dioxide(CeO_(2))powders was investigated through experiments and numerical simulations.In the experiment,CeO_(2)powder(average size of 30μm)was injected into radio-frequency(RF...The in-flight heating process of cerium dioxide(CeO_(2))powders was investigated through experiments and numerical simulations.In the experiment,CeO_(2)powder(average size of 30μm)was injected into radio-frequency(RF)argon plasma,and the temperatures were measured using a DPV-2000 monitor.A model combining the electromagnetism,thermal flow,and heat transfer characteristics of powder during in-flight heating in argon plasma was proposed.The melting processes of CeO_(2)powders of different diameters,with and without thermal resistance effect,were investigated.Results show that the heating process of CeO_(2)powder particles consists of three main stages,one of which is relevant to a dimensionless parameter known as the Biot number.When the Biot value≥0.1,thermal resistance increases significantly,especially for the larger powders.The predicted temperature of the particles at the outlet(1800–2880 K)is in good agreement with the experimental result.展开更多
基金financially supported by National Natural Science Foundation of China(22466010)Guizhou Provincial Basic Research Program(Natural Science)ZK[2023]47 and key program ZD[2025]075+6 种基金Innovation and Entrepreneurship Project for overseas Talents in Guizhou Province[2022]02Specific Natural Science Foundation of Guizhou University(X202207)the national undergraduate innovation and entrepreneurship training program(gzugc2023006gzusc2024012)SRT project of Guizhou university(2023SRT0292023SRT024)supported by Shanghai Technical Service Center of Science and Engineering Computing,Shanghai University。
文摘Electrocatalytic nitrate reduction reaction(NO3RR)represents a sustainable and environmentally benign route for ammonia(NH3)synthesis.However,NO3RR is still limited by the competition from hydrogen evolution reaction(HER)and the high energy barrier in the hydrogenation step of nitrogen-containing intermediates.Here,we report a selective etching strategy to construct Ru M nanoalloys(M=Fe,Co,Ni,Cu)uniformly dispersed on porous nitrogen-doped carbon substrates for efficient neutral NH3electrosynthesis.Density functional theory calculations confirm that the synergic effect between Ru and transition metal M modulates the electronic structure of the alloy,significantly lowering the energy barrier for the conversion of*NO_(2)to*HNO_(2).Experimentally,the optimized Ru Fe-NC catalyst achieves 100%Faraday efficiency with a high yield rate of 0.83 mg h^(-1)mg^(-1)catat a low potential of-0.1 V vs.RHE,outperforming most reported catalysts.In situ spectroscopic analyses further demonstrate that the Ru M-NC effectively promotes the hydrogenation of nitrogen intermediates while inhibiting the formation of hydrogen radicals,thereby reducing HER competition.The Ru FeNC assembled Zn-NO_(3)^(-)battery achieved a high open-circuit voltage and an outstanding power density and capacity,which drive selective NO_(3)^(-)conversion to NH3.This work provides a powerful synergistic design strategy for efficient NH3electrosynthesis and a general framework for the development of advanced multi-component catalysts for sustainable nitrogen conversion.
基金supported by the National Natural Science Foundation of China(52402298,52172224,52302240)Science and Technology Correspondent Project of Tianjin(24YDTPJC00240)+1 种基金the Macao Young Scholars Program(AM2023011)the Yuanguang Scholars Program,Hebei University of Technology(282022554).
文摘Zinc telluride(ZnTe)with high density and low cost is considered as promising anode for sodium-ion batteries.However,ZnTe suffers from continuous capacity degradation owing to the low electronic conductivity,large volume expansion,and high ion-diffusion energy barriers.Herein,the nitrogen-doped carbon confined ZnTe polyhedron heterostructure(ZnTe/NC)is proposed,exploiting its orbital rehybridization and the realignment of energy level to improve storage performance.Systematic ex situ/in situ characterizations and simulations demonstrated that the elaborate ZnTe/NC offers abundant electron/ion transport pathways,accelerates Na^(+)diffusion kinetics,and alleviates huge volume expansion.Notably,the nitrogen-doped carbon-support interaction induced via electron transfer between ZnTe sites and support elevates the energy level of Zn 3d orbital,greatly enhancing ion adsorption capability and reducing the ion diffusion barrier.As a result,the ZnTe/NC anode delivers a high discharge capacity of 470.5 mAh g^(−1)and long cycling durability over 1000 cycles.This work uncovers that optimizing sodium ion adsorption and diffusion via d-orbital energy level modulation enabled by nitrogen-doped support interaction is an effective method for developing high-performance transition metal telluride anodes for alkali ion storage.
文摘Nitrogen doping is a promising way to modulate the electrical properties of graphene to realize graphene-based electronics and promise fascinating properties and applications.Herein,we report a method to noncovalently assembly titanium(Ⅳ) bis(ammoniumlactato) dihydroxide(Ti complex) on nitrogen-doped graphene to create a reliable hybrids which can be used as a reversible chemical induced switching.As the adsorption and desorption of Ti complex in sequential treatments,the conductance of the nitrogen-doped graphene transistors was finely modulated.Control experiments with pristine graphene clearly demonstrated the important effort of the nitrogen in this chemical sensor.Under optimized conditions,nitrogen-doped graphene transistors open up new ways to develop multifunctional devices with high sensitivity.
基金supported by the Science and Technology Development Foundation of Pudong New Area (No.PKJ2014Z03)Dawn Program of Shanghai (No.09SG54)+1 种基金Material Science and Engineering Key Subject of Shanghai Polytechnic University (No.XXKZD1601)Gaoyuan Discipline of Shanghai-Environmental Science and Engineering (Resource Recycling Science and Engineering)
文摘Phosphate residue is regarded as a hazardous waste, which could potentially create significant environmental and health problems if it is not properly treated and disposed of. In this study, nitrogen-doped carbon nanotubes-FePO_4(NCNTs-FePO_4) composite was successfully synthesized from phosphate residue, and its application as an effective catalyst was explored. Firstly, an effective method was developed to recover FePO_4 from phosphate residue, achieving an impressive FePO_4 mass recovery rate of 98.14%. Then, the NCNTsFePO_4 catalyst was synthesized from the recovered FePO_4 by two main reactions, including surface modification and chemical vapor deposition. Finally, the synthesized NCNTs-FePO_4 was applied to photo-degrade 15 mg/L Rhodamine B(RhB) in a Fenton-like system. The results showed that 98.9% of RhB could be degraded in 60 min, closely following the pseudofirst-order kinetics model. It was found that even after six consecutive cycles, NCNTs-FePO_4 still retained a high catalytic capacity(>50%). Moreover, ·OH radicals participating in the RhB degradation process were evidenced using quenching experiments and electron paramagnetic resonance analysis, and a rational mechanism was proposed. It was demonstrated that the materials synthesized from hazardous phosphate residue can be used as an effective catalyst for dye removal.
基金supported by the National Natural Science Foundation of China(21476087,21576101)the Innovation Project of Guangdong Department of Education(2014KTSCX016)+1 种基金the Science&Technology Research Project of Guangdong Province(2013B010405005,2014A010105041)the Fundamental Research Funds for the Central Universities~~
文摘Aniline,pyrrole and phenanthroline,which have different nitrogen compositions,are used as carbon precursors to synthesize nitrogen-doped ordered mesoporous carbons（NOMCs） by the nanocasting method.The effect of the precursor on the resultant NOMC is extensively investigated by nitrogen adsorption-desorption measurements,scanning electron microscopy,X-ray photoelectron spectroscopy（XPS）,cyclic voltammetry and rotating ring-disk electrode measurements.Salient findings are as follows.First,the precursor has a significant influence on the specific surface area and textural properties.The NOMC materials derived from pyrrole（C-PY-900：765 m^2/） and phenanthroline（C-Phen-900：746 m^2/） exhibit higher specific surface areas than the aniline analog（C-PA-900：569 m^2/）.Second,the XPS results indicate that the total nitrogen content（ca.3.1–3.3 at%） is similar for the three carbon sources,except for a slight difference in the nitrogen configuration.Furthermore,the content of the nitrogen-activated carbon atoms is found to closely depend on the precursor,which is the highest for the phenanthroline-derived carbon.Third,the electrochemical results reveal that the electrocatalytic activity follows in the order C-PA-900 C-PY-900 C-Phen-900,confirming that the nitrogen-activated carbon atoms are the active sites for the oxygen reduction reaction（ORR）.In summary,the precursor has considerable influence on the composition and textural properties of the NOMC materials,of which the ORR electrocatalytic activity can be enhanced through optimization of the NOMCs.
基金supported by the Open Research Fund Program of Engineering Technology Research Center of Coal Resources Comprehensive Utilization,Anhui Province,Anhui University of Science and Technology(Grant No.MTYJZX202301)the Anhui Provincial Natural Science Foundation(Grant No.2008085J27).
文摘Traditionally reduced graphene oxide(RGO)-based electromagnetic wave(EMW)absorbing materials have poor absorption effectiveness due to impedance mismatch caused by skin effect.The introduction of structural defects and the design of heterogeneous interfaces play a crucial role in enhancing the polarization effect of EMW absorbers.In this study,nitrogen-doped reduced graphene oxide/zinc ferrite@nitrogen-doped carbon(NRGO/ZnFe_(2)O_(4)@NC)ternary composite with rich heterogeneous interfaces is constructed by combining solvothermal reaction,in-situ polymerization,annealing treatment with subsequent hydrothermal reaction.The research results have shown that the obtained NRGO/ZnFe_(2)O_(4)@NC ternary composite exhibits a unique core-shell structure and excellent EMW absorption performance.At a thickness of 2.61 mm,the maximum effective absorption bandwidth can reach 7.2 GHz,spanning the entire Ku-band and a portion of the X-band,and the minimum reflection loss is-61.1 dB,which is superior to most reported RGO-based EMW absorbers.The excellent EMW absorbing ability is mainly ascribed to the optimized impedance matching and the enhanced polarization loss caused by the abundant heterogeneous interfaces and structural defects derived from heteroatomic nitrogen doping.Furthermore,the radar cross section in the far field is simulated by a computer simulation technique.This study provides a novel way to prepare core-shell magnetic carbon composites as highly efficient and broadband EMW absorbers.
基金supported by the Synchrotron Light Research Institute(Public Organization)Thailand(GS-54-D01)+7 种基金the Commission on Higher EducationMinistry of EducationThailandperformed under the project"Sustainable Chemical Synthesis(Sus Chem Sys)"which is co-financed by the European Regional Development Fund(ERDF)the state of North Rhine-WestphaliaGermanyunder the Operational Programme"Regional Competitiveness and Employment"2007–2013
文摘Nitrogen-doped carbon nanotubes （NCNTs） were used as a support for iron （Fe） nanoparticles applied in car- bon dioxide （CO_2） hydrogenation at 633 K and 25 bar （1 bar = 10-5 Pa）. The Fe/NCNT catalyst promoted with both potassium （K） and manganese （Mn） showed high performance in CO_2 hydrogenation, reaching 34.9% conversion with a gas hourly space velocity （GHSV） of 3.1 L-（g·h）-1. Product selectivities were high for olefin products and low for short-chain alkanes for the K-promoted catalysts. When Fe/NCNT catalyst was promot- ed with both K and Mn, the catalytic activity was stable for 60 h of reaction time. The structural effect of the Mn promoter was demonstrated by X-ray diffraction （XRD）, temperature-programmed reduction （TPR） with molecular hydrogen （H2）, and in situ X-ray absorption near-edge structure （XANES） analysis. The Mn pro- moter stabilized wtistite （FeO） as an intermediate and lowered the TPR onset temperature. Catalytic ammo- nia （NH_3） decomposition was used as an additional probe reaction for characterizing the promoter effects. The Fe/NCNT catalyst promoted with both K and Mn had the highest catalytic activity, and the Mn-promoted Fe/NCNT catalysts had the highest thermal stability under reducing conditions.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.22278092,22078116 and 22222805)Guangdong Provincial Key Research and Development Program(No.2020B1111380002)+2 种基金Science and Technology Research Project of Guangzhou(Nos.2023A03J0034,2023A04J0077 and 202102020467)State Key Laboratory of Pulp and Paper Engineering(No.202313)Key Discipline of Materials Science and Engineering,Bureau of Education of Guangzhou(No.202255464).
文摘Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NHMC/Ni/NiO)nanocomposite for developing high-capacity LIBs anode materials through carbonization and selective etching strategies.The synthesized NMHC/Ni/NiO-0.33 composite exhibited a highly regular microstructure with well-dispersed Ni/NiO particles.The composite had a surface area of 408 m^(2)·g^(−1),a mesopore ratio of 75.0%,and a pyridine–nitrogen ratio of 58.9%.The introduction of nitrogen atoms reduced the disordered structure of lignin mesoporous carbon and enhanced its electrical conductivity,thus improving the lithium storage capabilities of the composite.Following 100 cycles at a current density of 0.2 A·g^(−1),the composite demonstrated enhanced Coulomb efficiency and rate performance,achieving a specific discharge capacity of 1230.9 mAh·g^(−1).At a high-current density of 1 A·g^(−1),the composite exhibited an excellent specific discharge capacity of 714.6 mAh·g^(−1).This study presents an innovative method for synthesizing high-performance anode materials of LIBs.
基金supported by Zhejiang Provincial Natural Science Foundation(No. LY21B070005)National Undergraduate Training Program for Innovation and Entrepreneurship of China(Nos. 202110345015 and 202110345016)Self designed scientific research project of Zhejiang Normal University(No. 2021ZS06)。
文摘In this report, nitrogen-doped porous carbons were synthesized from polyacrylonitrile fiber by a facile two-step synthesis process i.e. carbonization followed by KOH activation. Activation temperature and KOH/carbon ratio are two parameters to tune the porosity and surface chemical properties of sorbents. The as-obtained sorbents were carefully characterized.Special attention was paid concerning the change of sorbents’ morphology with respect to synthesis conditions. Under the activation temperatures of this study, the sorbents can still retain their fibrous structure when the KOH/carbon mass ratio is 1. Further increasing the KOH amount will destroy the original morphology of polyacrylonitrile fiber. CO_(2)adsorption performance tests show that a sorbent retaining the fibrous shape possesses the highest CO_(2)uptake of 3.95 mmol/g at 25℃and 1 bar. Comprehensive investigation found that the mutual effect of narrow microporosity and doped N content govern the CO_(2)adsorption capacity of these adsorbents. Furthermore, these polyacrylonitrile fiber-derived carbons present multiple outstanding CO_(2)capture properties such as excellent recyclability, high CO_(2)/N_(2)selectivity, fast adsorption kinetics, suitable heat of adsorption, and good dynamic adsorption capacity. Hence, nitrogen-doped porous carbons with fibrous structure are promising in CO_(2)capture.
基金National Natural Science Foundation of China(T2188101)。
文摘Among the synthesis techniques for graphene,chemical vapor deposition(CVD)enables the direct growth of graphene films on insulating substrates.Its advantages include uniform coverage,high quality,scalability,and compatibility with industrial processes.Graphene is chemically inert and has a zero-bandgap which poses a problem for its use as a functional layer,and nitrogen doping has become an important way to overcome this.Post-plasma treatment has been explored for the synthesis of nitrogen-doped graphene,but the procedures are intricate and not suitable for large-scale production.We report the direct synthesis of nitrogen-doped graphene on a 4-inch sapphire wafer by ethanol-assisted CVD employing pyridine as the carbon feedstock,where the nitrogen comes from the pyridine and the hydroxyl group in ethanol improves the quality of the graphene produced.Additionally,the types of nitrogen dopant produced and their effects on III-nitride epitaxy were also investigated,resulting in the successful illumination of LED devices.This work presents an effective synthesis strategy for the preparation of nitrogen-doped graphene,and provides a foundation for designing graphene functional layers in optoelectronic devices.
文摘The most energy-inefficient step in the oxygen evolution reaction(OER), which involves a complicated four-electron transfer process, limits the efficiency of the electrochemical water splitting. Here, well-defined Ni/Co3O4 nanoparticles coupled with N-doped carbon hybrids(Ni/Co3O4@NC) were synthesized via a facile impregnation-calcination method as efficient electrocatalysts for OER in alkaline media. Notably, the impregnation of the polymer with Ni and Co ions in the first step ensured the homogeneous distribution of metals, thus guaranteeing the subsequent in situ calcination reaction, which produced well-dispersed Ni and Co3O4 nanoparticles. Moreover, the N-doped carbon matrix formed at high temperatures could effectively prevent the aggregation and coalescence, and regulate the electronic configuration of active species. Benefiting from the synergistic effect between the Ni, Co3O4, and NC species, the obtained Ni/Co3O4@NC hybrids exhibited enhanced OER activities and remarkable stability in an alkaline solution with a smaller overpotential of 350 m V to afford 10 m A cm-2, lower Tafel slope of 52.27 m V dec-1, smaller charge-transfer resistance, and higher double-layer capacitance of 25.53 m F cm-2 compared to those of unary Co3O4@NC or Ni@NC metal hybrids. Therefore, this paper presents a facile strategy for designing other heteroatom-doped oxides coupled with ideal carbon materials as electrocatalysts for the OER.
基金financial support from the NSFC(Grant No.21403119)the Science and Technology Bureau of Shenzhen(Grant No.JCYJ20170306171540744)
文摘Non-noble metal electrocatalysis has witnessed rapid and profound performance improvements owing to the emergence of advanced nanosynthetic techniques.Integration of these nanotechniques can lead to synergistic performance enhancement,but such system-engineering strategies are difficult to achieve because of the lack of effective synthesis method.We hereby demonstrate an integrated approach that combines most of the existing nanotechniques in a facile one-pot synthesis.Material characterization reveals that the product shows key features intended by techniques including morphological,structural,doping,heterointerface,and surface wetting engineering.The as-obtained nitrogen-doped hierarchical heterostructured MoS_(x)/Ni_(3)S_(2)nanowires show an overpotential that is only50 mV higher than commercial Pt/C for hydrogen evolution reaction over current densities from 10 to 150 mA cm^(-2).Correlations between the adopted nanotechniques and the electrochemical reaction rates are established by evaluating the impacts of individual techniques on the activation energy,pre-exponential factor,and transfer coefficient.This indepth analysis provides a full account of the synergistic effects and the overall improvement in electrocatalytic performance of hydrogen evolution reaction.This work manifests a generic strategy for multipurpose material design in non-noble metal electrocatalysis.
基金supported by the National Natural Science Foundation of China(21503264,22179081 and 22076117)Natural Science Foundation of Shanghai(20ZR1422500).
文摘We synthesized CN11,a carbon nitride material rich in sp^(3)hybrid graphitic nitrogen(sp^(3)-N),employing a facile oxalic acid-assisted melamine molecular assembly strategy.CN11 promoted the formation of Pd nanoparticles(NPs)predominantly exposing{200}facets,termed Pd/CN11-2.This facet-specific configuration significantly boosted hydrogen adsorption,leading to notable improvements in catalytic activity.Compared to Pd/XC-72-2 and Pd/g-C_(3)N_(4)-2,Pd/CN11-2 exhibited a remarkable two-fold and nineteen-fold increase in catalytic yield for hydrazo compound hydrogenation,respectively.Pd/CN11-2 also demonstrated robust performance across a range of reaction conditions,maintaining excellent yield.This study emphasizes the critical role of tailored support structures in controlling Pd NPs facets,thereby enhancing hydrogenation efficiency.It provides valuable insights for advancing the industrial application of Pd-based catalysts,underscoring the importance of strategic support modulation for optimizing catalytic performance.
文摘Development of efficient and stable metal catalysts for the selective aqueous phase hydrodeoxygenation(HDO)of biomass-derived oxygenates to value-added biofuels is highly desired.An innovative surface microenvironment modulation strategy was used to construct the nitrogen-doped hollow carbon sphere encapsulated with Pd(Pd@NHCS-X,X:600–800)nanoreactors for catalytic HDO of biomass-derived vanillin in water.The specific surface microenvironments of Pd@NHCS catalysts including the electronic property of active Pd centers and the surface wettability and porous structure of NHCS supports could be well-controlled by the calcination temperature of catalysts.Intrinsic kinetic evaluations demonstrated that the Pd@NHCS-600 catalyst presented a high turnover frequency of 337.77 h^(–1)and a low apparent activation energy of 18.63 kJ/mol.The excellent catalytic HDO performance was attributed to the unique surface microenvironment of Pd@NHCS catalyst based on structure-performance relationship analysis and DFT calculations.It revealed that pyridinic N species dominated the electronic property regulation of Pd sites through electronic metal-support interaction(EMSI)and produced numerous electron-rich active Pd centers,which not only intensified the dissociation and activation of H2 molecules,but also substantially improved the activation capability of vanillin via the enhanced adsorption of–C=O group.The fine hydrophilicity and abundant porous structure promoted the uniform dispersion of catalyst and ensured the effective access of reactants to catalytic active centers in water.Additionally,the Pd@NHCS-600 catalyst exhibited excellent catalytic stability and broad substrate applicability for the selective aqueous phase HDO of various biomass-derived carbonyl compounds.The proposed surface microenvironment modulation strategy will provide a new consideration for the rational design of high-performance nitrogen-doped carbon-supported metal catalysts for catalytic biomass transformation.
基金partially supported by the National Natural Science Foundation of China(No.22373092,No.22288201)CAS Project for Young Scientists in Basic Research(YSBR-051)supported by USTC Tang Scholarship。
文摘Utilizing nitrate(NO_(3)^(-))as the nitrogen source to produce ammonia can effectively remove NO_(3)^(-)pollutant while obtaining valuable ammonia,and the understanding of the mechanisms is essential for the design of new catalysts.In this work,by using density functional theory calculations,the electroreduction mechanisms of nitrate reduction reaction(NO_(3)RR)on transition metal single atom supported on 3N-coordinated N-doped graphene(TM/N_(3)-G)are systematically investigated.It is found that the protonation of ^(*)OH acts as the potential determing steps except for the traditionally considered ^(*)NO_(3)/^(*)NO/^(*)NO_(2) protonation step and the desorption of water may play an important role for NO_(3)RR on some TM/N_(3)-G.By considering the stability of single-atom catalyst(SAC),the preferential adsorption of NO_(3)^(-)larger than H and H_(2)O,the limiting potential of whole NO_(3)RR,the selectivity toward NH3,V(Mn,Os)/pyrrolic-N_(3)-G and Mn(Ru,Ir)/pyridinic-N_(3)-G are screened out as potential SACs for NO_(3)RR.This work provides an understanding of the NO_(3)RR mechanism and highlights several promising NO_(3)RR catalysts based on the TM/N_(3)-G system.
基金sponsored by the National Natural Science Foundation of China(Nos.U23A6005 and 22178069)。
文摘Zn-air battery(ZAB)has garnered significant attention owing to its environmental friendliness and safety attributes.A critical challenge in advancing ZAB technology lies in the development of high-performance and cost-effective electrocatalysts for oxygen redox reactions(OER and ORR).Herein,we report Co/Fe carbon-supported composites as efficient bifunctional catalyst encapsulated in oxidative ammonolysis modified lignin-derived N-doped biochar(Co Fe-Co_(x)N@NOALC).It exhibited exceptional electrochemical performance in aqueous ZAB owing to their uniform dispersed and small particle size,with a peak power density of 154 mW/cm^(2)and a specific capacity of 770 mAh/g.Most notably,it exhibited a long cycle stability,surpassing 1500 h at a current density of 10 mA/cm^(2),with a mere 11.4%decrease in the chargedischarge efficiency of the battery.This study proposes a viable strategy for enhancing the performance and reducing the cost of Zn-air batteries through the utilization of biomass-derived materials.
基金supported by the National Key Technologies R&D Program of China(Nos.2022YFE0114800 and 2021YFA1502100)National Natural Science Foundation of China(Nos.22075047,22032002,U1905214,21961142019)the 111 Project(Nos.D16008)。
文摘Solar-induced water oxidation reaction(WOR)for oxygen evolution is a critical step in the transformation of Earth's atmosphere from a reducing to an oxidation one during its primordial stages.WOR is also associated with important reduction reactions,such as oxygen reduction reaction(ORR),which leads to the production of hydrogen peroxide(H_(2)O_(2)).These transitions are instrumental in the emergence and evolution of life.In this study,transition metals were loaded onto nitrogen-doped carbon(NDC)prepared under the primitive Earth's atmospheric conditions.These metal-loaded NDC samples were found to catalyze both WOR and ORR under light illumination.The chemical pathways initiated by the pristine and metal-loaded NDC were investigated.This study provides valuable insights into potential mechanisms relevant to the early evolution of our planet.
基金supported by the National Natural Science Foundation of China(Grant Nos.51272237,51272231,and 51010002)the China Postdoctoral Science Foundation(Grant Nos.2012M520063,2013T60587,and Bsh1201016)
文摘Nitrogen-doped diamond-like carbon （DLC：N） films prepared by the filtered cathodic vacuum arc technology are functionalized with various chemical molecules including dopamine （DA）, 3-Aminobenzeneboronic acid （APBA）, and adenosine triphosphate （ATP）, and the impacts of surface functionalities on the surface morphologies, compositions, microstructures, and cell compatibility of the DLC：N films are systematically investigated. We demonstrate that the surface groups of DLC：N have a significant effect on the surface and structural properties of the film. The activity of PC12 cells depends on the particular type of surface functional groups of DLC：N films regardless of surface roughness and wettability. Our research offers a novel way for designing functionalized carbon films as tailorable substrates for biosensors and biomedical engineering applications.
基金supported by the National Natural Science Foundation of China(Grant No.22276123,22025505)the Oceanic Interdisciplinary Program of Shanghai Jiao Tong University(SL2022ZD105)State Key Lab of Metal Matrix Composite。
文摘The recycling of plastics is a significant global concern.Due to the thermosetting properties of melamineformaldehyde(MF)resin plastics,which make heating and melting difficult,their recycling and reuse pose substantial challenges.In this study,we developed nitrogen-doped(N-doped)carbon materials through scalable carbonization of MF resin plastic waste.This metal-free N-doped carbon catalyst achieved a hydrogen peroxide(H_(2)O_(2))production rate of 971.6 mmol gcatalyst^(-1)h^(-1)with a Faradaic efficiency for H_(2)O_(2)(FEH_(2)O_(2))exceeding 90%under acidic conditions.Additionally,a flow cell utilizing this carbon catalyst demonstrated a production rate of 11.3 mol cm^(-2)h^(-1)(22.5 mol g_(catalyst)^(-1)h^(-1))and maintained a record-high current density of approximately 530 mA cm^(-2)over 300 h.In-situ electrochemical surface-enhanced Raman spectroscopy and density functional theory calculations revealed the presence of porphyrin-like carbon defects,which serve as active sites for the continuous and stable generation of^(*)OOH species.The nitrogen-doped carbon materials obtained from large-scale carbonization of MF plastic waste exhibit abundant active sites,making them highly promising electrocatalysts for the two-electron oxygen reduction reaction(2e^(-)ORR).
基金National Natural Science Foundation of China(11875039)Shanxi Scholarship Council of China(2023-033)+2 种基金Fundamental Research Program of Shanxi Province(202303021221071)China Baowu Low Carbon Metallurgical Innovation Foundation(2022)2023 Anhui Major Industrial Innovation Plan Project。
文摘The in-flight heating process of cerium dioxide(CeO_(2))powders was investigated through experiments and numerical simulations.In the experiment,CeO_(2)powder(average size of 30μm)was injected into radio-frequency(RF)argon plasma,and the temperatures were measured using a DPV-2000 monitor.A model combining the electromagnetism,thermal flow,and heat transfer characteristics of powder during in-flight heating in argon plasma was proposed.The melting processes of CeO_(2)powders of different diameters,with and without thermal resistance effect,were investigated.Results show that the heating process of CeO_(2)powder particles consists of three main stages,one of which is relevant to a dimensionless parameter known as the Biot number.When the Biot value≥0.1,thermal resistance increases significantly,especially for the larger powders.The predicted temperature of the particles at the outlet(1800–2880 K)is in good agreement with the experimental result.
