Electrically conductive elastomer composites(CECs)with segregated networks of conductive nanofillers show high potential in stretchable strain sensors due to balanced mechanical and electrical properties,yet the sensi...Electrically conductive elastomer composites(CECs)with segregated networks of conductive nanofillers show high potential in stretchable strain sensors due to balanced mechanical and electrical properties,yet the sensitivity at low strain is generally insufficient for practical application.Herein,we report an easy and effective way to improve the resistive response to low strain for CECs with segregated network structure via adding stiff alumina into carbon nanostructures(CNS).The CEC containing 0.7 wt%CNS and 5 wt%Al_(2)O_(3) almost sustains the same elasticity(elongation at break of~900%)and conductivity(0.8 S/m)as the control,while the piezoresistive sensitivity is significantly improved.Thermoplastic polyurethane(TPU)composites with a segregated network of hybrid nanofillers(CNS and Al_(2)O_(3))show much higher strain sensitivity(Gauge factor,GF-566)at low strain(45%strain)due to a local stress concentration effect,this sensitivity is superior to that of TPU/CNS composites(GF-11).Such a local stress concentration effect depends on alumina content and its distribution at the TPU particle interface.In addition,CECs with hybrid fillers show better reproducibility in cyclic piezoresistive behavior testing than the control.This work offers an easy method for fabricating CECs with a segregated filler network offering stretchable strain sensors with a high strain sensitivity.展开更多
The effect of synthesized nanostructures,including graphene oxide,chemically reduced graphene oxide with sodium dodecyl sulfate(SDS),chemically reduced graphene oxide with polyvinylpyrrolidone,and multi-walled carbon ...The effect of synthesized nanostructures,including graphene oxide,chemically reduced graphene oxide with sodium dodecyl sulfate(SDS),chemically reduced graphene oxide with polyvinylpyrrolidone,and multi-walled carbon nanotubes,on the kinetics of methane hydrate formation was investigated in this work.The experiments were carried out at a pressure of 4.5 MPa and a temperature of 0 ℃ in a batch reactor.By adding nanostructures,the induction time decreases,and the shortest induction time appeares at certain concentrations of reduced graphene oxide with SDS and graphene oxide,that is,at a concentration of 360 ppm for reduced graphene oxide with SDS and 180 ppm for graphene oxide,with a 98% decrease in induction time compared to that in pure water.Moreover,utilization of carbon nanostructures increases the amount and the rate of methane consumed during the hydrate formation process.Utilization of multi-walled carbon nanotubes with a concentration of 90 ppm showes the highest amount of methane consumption.The amount of methane consumption increases by 173% in comparison with that in pure water.The addition of carbon nanostructures does not change the storage capacity of methane hydrate in the hydrate formation process,while the percentage of water conversion to hydrate in the presence of carbon nanotubes increases considerably,the greatest value of which occurres at a 90 ppm concentration of carbon nanotubes,that is,a 253% increase in the presence of carbon nanotubes compared to that of pure water.展开更多
A strong interface coupling is of vital importance to develop metal oxide/carbon nanocomposite anodes for next-generation lithium ion batteries.Herein,a rational N-doped carb on riveting strategy is designed to boost ...A strong interface coupling is of vital importance to develop metal oxide/carbon nanocomposite anodes for next-generation lithium ion batteries.Herein,a rational N-doped carb on riveting strategy is designed to boost the lithium storage performance of Fe3O4/N-doped carbon tubular structures.Poly pyrrole(PPy)has been used as the precursor for N-doped carbon.N-doped carbon-riveted Fe3O4/N-doped carbon(N-C@Fe3O4@N-C)nanocomposites were obtained by pyrolysis of PPy-coated FeOOH@PPy nanotubes in Ar atmosphere.When tested as an anode for LIBs,the N-C@Fe3O4@N-C displays a high reversible discharge capacity of 675.8 mA h g-1 after 100 cycles at a current density of 100 mA g-1 and very good rate capability(470 mA h g_1 at 2 A g-1),which significantly surpasses the performance of Fe3O4@N-C.TEM analysis reveals that after battery cycling the FeOx particles detached from the carbon fibers for Fe3O4@N-C,while for N-C@Fe3O4@N-C the FeOx particles were still trapped in the carbon matrix,thus preserving good electrical contact.Consequently,the superior performance of N-C@Fe3C)4@N-C is attributed to the synergistic effect between Fe3O4 and N-doped carbon combined with the unique structure properties of the nanocomposites.The strategy reported in this work is expected to be applicable for designing other electrode materials for LIBs.展开更多
The burgeoning global economy during the past decades gives rise to the continuous increase in fossil fuels consumption and rapid growth of CO_(2) emission,which demands an urgent exploration into green and sustainabl...The burgeoning global economy during the past decades gives rise to the continuous increase in fossil fuels consumption and rapid growth of CO_(2) emission,which demands an urgent exploration into green and sustainable devices for energy storage and power management.Supercapacitors based on activated carbon electrodes are promising systems for highly efficient energy harvesting and power supply,but their promotion is hindered by the moderate energy density compared with batteries.Therefore,scalable conversion of CO_(2) into novel carbon nanostructures offers a powerful alternative to tackle both issues:mitigating the greenhouse effect caused by redundant atmospheric CO_(2) and providing carbon materials with enhanced electrochemical performances.In this tutorial review,the techniques,opportunities and barriers in the design and fabrication of advanced carbon materials using CO_(2) as feedstock as well as their impact on the energy-storage performances of supercapacitors are critically examined.In particular,the chemical aspects of various Cv2 conversion reactions are highlighted to establish a detailed understanding for the science and technology involved in the microstructural evolution,surface engineering and porosity control of CO_(2)-converted carbon nanostructures.Finally,the prospects and challenges associated with the industrialization of CO_(2) conversion and their practical application in supercapacitors are also discussed.展开更多
Covalent organic frameworks(COFs)after undergoing the superlithiation process promise high-capacity anodes while suffering from sluggish reaction kinetics and low electrochemical utilization of redox-active sites.Here...Covalent organic frameworks(COFs)after undergoing the superlithiation process promise high-capacity anodes while suffering from sluggish reaction kinetics and low electrochemical utilization of redox-active sites.Herein,integrating carbon nanotubes(CNTs)with imine-linked covalent organic frameworks(COFs)was rationally executed by in-situ Schiff-base condensation between 1,1′-biphenyl]-3,3′,5,5′-tetracarbaldehyde and 1,4-diaminobenzene in the presence of CNTs to produce core–shell heterostructured composites(CNT@COF).Accordingly,the redox-active shell of COF nanoparticles around one-dimensional conductive CNTs synergistically creates robust three-dimensional hybrid architectures with high specific surface area,thus promoting electron transport and affording abundant active functional groups accessible for electrochemical utilization throughout the whole electrode.Remarkably,upon the full activation with a superlithiation process,the as-fabricated CNT@COF anode achieves a specific capacity of 2324 mAh g^(−1),which is the highest specific capacity among organic electrode materials reported so far.Meanwhile,the superior rate capability and excellent cycling stability are also obtained.The redox reaction mechanisms for the COF moiety were further revealed by Fourier-transform infrared spectroscopy in conjunction with X-ray photoelectron spectroscopy,involving the reversible redox reactions between lithium ions and C=N groups and gradual electrochemical activation of the unsaturated C=C bonds within COFs.展开更多
We previously reported the direct electrochemical detection of insulin at bare carbon electrodes. Here a novel modified acetylene carbon black paste electrode(SiC/CB-CPE), based on the outstanding characteristics of s...We previously reported the direct electrochemical detection of insulin at bare carbon electrodes. Here a novel modified acetylene carbon black paste electrode(SiC/CB-CPE), based on the outstanding characteristics of silicon carbide nanostructure,was developed for the electrooxidation of insulin in alkaline solution and it was characterized by cyclic voltammetry(CV) and electrochemical impedance spectroscopy(EIS) in 5 mmol/L Fe(CN)63-/4- solution. It is found that silicon carbide nanostructure doped into the CB-CPE greatly facilitates the redox electrochemistry of Fe(CN)63-/4- probe and the electrochemical oxidation of insulin. The electrooxidation of insulin is a one-electron and one-proton reaction and an irreversible adsorption-controlled electrode process. The anodic oxidation current increases linearly with the concentration of insulin from 1×10-7mol/L to1.2×10-6mol/L in 0.1 mol/L Na2CO3-NaHCO3 buffer solution(pH 10.0) and the detection limit was 50 nmol/L. In addition, the SiC/CB-CPE shows good sensitivity, reproducibility, renewability and capacity of resisting disturbance.展开更多
The exploitation of renewable energy as well as the elimination of the harmful impact of excessive carbon emission are worldwide concerns for sustainable development of the ecological environment on earth.To address t...The exploitation of renewable energy as well as the elimination of the harmful impact of excessive carbon emission are worldwide concerns for sustainable development of the ecological environment on earth.To address that,the technologies regarding energy conversion systems,such as water splitting and electroreduction of carbon dioxide,have attracted significant attention for a few decades.Yet,to date,the production of green fuels and/or high energy density chemicals like hydrogen,methane,and ethanol,are still suffering from many drawbacks including high energy consumption,low selectivity,and sluggish reaction rate.In this regard,nanostructured bimetallic materials that is capable of taking the full benefits of the coupling effects between different elements/components with structure modification in nanoscale are considered as a promising strategy for high-performance electrocatalysts.Herein,this review aims to outline the important progress of these nanostructured bimetallic electrocatalysts.It starts with the introduction of some important fundamental background knowledge about the reaction mechanism to understand how these reactions happen.Subsequently,we summarize the most recent progress regarding how the nanostructured bimetallic electrocatalysts manipulate the activity and selectivity of catalytic reactions in the order of bimetallic alloying effect,interface/substrate effect of bi-component electrocatalyst,and nanostructuring effect.展开更多
The ability to control the nanoscale shape of carbon nanostructures during wide-scale synthesis process is an essential goal in research for Nanotechnology applications. This paper reports a significant progress towar...The ability to control the nanoscale shape of carbon nanostructures during wide-scale synthesis process is an essential goal in research for Nanotechnology applications. This paper reports a significant progress toward that goal. Variant CVD has been used for the synthesis of the samples studied. Curvature, hybridization and contamination are analyzed using Electron Microscopies and XANES spectroscopy. The investigations of the results show that four types of samples are obtained. They are carbon nanotubes (CNTs), carbon nanofibers (CNFs), carbon nanowalls (CNWs) and carbon nanoparticles (CNPs). Almost all of them have catalyst nanoparticles (metal) on top in top growth model or on base in base growth model and encapsulated or adsorbed in sidewalls. The orientation of tubular carbon nanomaterials depends on operating parameters. They are classified in three groups: the poorly oriented, the medium oriented and the highly oriented. Their contamination (radicals, atoms and molecules) and hybridization are intrinsically related to the curvature of their graphene layers. XANES spectroscopy allows quantitative characterization of nanomaterials.展开更多
An efficient method has been developed to synthesize well-aligned multi-walled carbon nanotubes (MWCNTs) on a conductive Ta substrate by chemical vapour deposition (CVD). Free-standing MWCNTs arrays were functionalize...An efficient method has been developed to synthesize well-aligned multi-walled carbon nanotubes (MWCNTs) on a conductive Ta substrate by chemical vapour deposition (CVD). Free-standing MWCNTs arrays were functionalized through electrochemical oxidation with the formation of hydroxyl and carboxyl functional groups. Using a new oven drying technique, we demonstrate that the unidirectionally aligned and laterally spaced geometry of the CNT arrays can be retained after being subjected to each step of electrochemical modification. Samples were analyzed by using a field emission scanning electron microscope (SEM), transmission electron microscope (TEM), Fourier transformed infrared (FTIR) and Raman spectroscopy. Useful electrochemical methods for the synthesis of various gold nanostructures onto the aligned MWCNTs were then presented for the first time. The results demonstrated that flowerlike nanoparticle arrays, nanosheets and nanoflowers were obtained on the aligned CNTs under different experimental conditions. These kinds of aligned-CNT/Au nanostructures hybrid materials introduced by these efficient and simple electrochemical methods could lead to development of a new generation device for ultrasensitive catalytic and biological application.展开更多
Natural rubber based composites containing different carbon nanofillers (fullerenes, carbon nanotubes (CNTs) and graphene nanoplatelets (GNPs)) at different concentrations have been prepared. Their dielectric properti...Natural rubber based composites containing different carbon nanofillers (fullerenes, carbon nanotubes (CNTs) and graphene nanoplatelets (GNPs)) at different concentrations have been prepared. Their dielectric properties (dielectric permittivity, dielectric loss) have been studied in the 1 - 12 GHz frequency range. Some factors (electromagnetic field frequency, fillers concentration, fillers intrinsic structure) influencing the dielectric behavior of the composites have been investigated. The dielectric properties of the developed natural rubber composites containing conductive fillers (fullerenes, CNTs, GNPs) indicate that these composites can be used as broadband microwave absorbing materials.展开更多
X-Ray Absorption Spectroscopy (XAS) on the carbon K edge of carbon nanostructures (nanotubes, nanofibers, nanowalls) is reported here. They are grown on plain SiO2 (8 nm thick)/Si(100) substrates by a Plasma and Hot F...X-Ray Absorption Spectroscopy (XAS) on the carbon K edge of carbon nanostructures (nanotubes, nanofibers, nanowalls) is reported here. They are grown on plain SiO2 (8 nm thick)/Si(100) substrates by a Plasma and Hot Filaments-enhanced Catalytic Chemical Vapor Deposition (PE HF CCVD) process. The morphology and the nature of these carbon nanostructures are characterized by SEM, TEM and Raman spectroscopy. According to conditions of catalyst preparation and DC HF CCVD process, carbon nanotubes (CNTs), carbon nanofibers (CNFs), carbon nanowalls (CNWs), carbon nanoparticles (CNPs) with different orientation of the graphene plans or shells can be prepared. From the angular dependence of the incident light and geometrical morphology of the nanostructures, wide variations of the C K-edge intensity of the transitions to the empty π* and σ* states occur. A full lineshape analysis of the XAS spectra has been carried out using a home-made software, allowing estimating the relative proportion of π* and σ* transitions. A geometrical model of the angular dependence with the incidence angle of the light and the morphology of the carbon nanostructures is derived. With normalization to the HOPG (Highly Oriented Pyrolytic Graphite graphite) reference case, a degree of alignment can be extracted which is representative of the localized orientation of the graphitic carbon π bonds, accounting not only for the overall orientation, but also for local defects like impurities incorporation, structural defects ... This degree of alignment shows good agreement with SEM observations. Thus CNTs films display degrees of alignment around 50%, depending on the occurrence of defects in the course of the growth, whereas no special alignment can be detected with CNFs and CNPs, and a weak one (about 20%) is detected on CNWs.展开更多
VS_(4) has a unique layered atomic chain structure and has the potential to become a high-performance cathode material of magnesium-ion batteries with a high capacity and long cycle life.However,low conductivity and s...VS_(4) has a unique layered atomic chain structure and has the potential to become a high-performance cathode material of magnesium-ion batteries with a high capacity and long cycle life.However,low conductivity and sluggish Mg^(2+)diffusivity during cycling limit its practical application in large-scale energy storage.Herein,a cooperative assembly-directed strategy is adopted to synthesize VS_(4) nanorods grown in situ on carbon nanotubes(CNTs/VS_(4)).VS_(4) nanorods are tightly anchored to CNTs through V-O-C interface covalent bonds,and CNTs can enhance the electronic conductivity of the nanocomposite.In addition,the ion insertion reaction using Mg^(2+)and Mg Cl^(+)as carriers reduces the polar barrier for divalent Mg^(2+)ion transport.This rationally designed architecture promotes ion diffusion and electron transfer,thus facilitating reaction kinetics.The cooperative assembly-oriented strategy can endow CNTs/VS_(4) with excellent magnesium storage properties,including a high reversible capacity of 223.2 m Ah g^(-1)at a current density of 50 m A g^(-1),a remarkable discharge capacity of 91.8 m Ah g^(-1)even at 2,000 m A g^(-1),and an impressive capacity retention of 85.2% after 1,000 cycles at 500 m A g^(-1).Moreover,this strategy can serve as a general synthetic method for the complexation of VS_(4) with other carbon nanostructures.展开更多
An extensive study of Fischer-Tropsch synthesis on nanostructure supports with high surface area such as nanostructure -y-alumina, single wall carbon nanotubes (SWNTs), and the hybrid of SWNTs/nanostructure -y-alumi...An extensive study of Fischer-Tropsch synthesis on nanostructure supports with high surface area such as nanostructure -y-alumina, single wall carbon nanotubes (SWNTs), and the hybrid of SWNTs/nanostructure -y-alumina has been investigated. The nanostructure γ-alumina was promoted with lanthanum to obtain better performance of catalyst and 15 wt% cobalt loading was the basis of our investigation. Fischer- Tropsch synthesis was performed in a fixed bed reactor under different reaction conditions (220-240 ℃, 15-25 bar, H2/CO ratio of 2, GHSV of 900-1400) in order to study the effects of temperature, pressure and gas hourly space velocity (GHSV) changes on hydrocarbon selec- tivity and catalyst activity. The catalysts were extensively characterized by different methods including X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), inductively coupled plasma (ICP), hydrogen (H2) chemisorption and temperature-programmed reduction (TPR). The results showed that the yield of hybrid supported catalyst (55.4%) is higher than that of nanos- tructure -y-alumina supported catalyst (55.0%) and lower than that of SWNTs supported cobalt catalyst (71.0%). The hybrid supported catalyst showed higher reduction degree and dispersion of cobalt particles. The temperature, pressure and GHSV effects on hybrid supported catalyst were studied and results showed that higher pressure favors the chain growth and temperature increase leads to the increases in methane selec- tivity and CO conversion. Higher hydrocarbon selectivity and CO conversion showed positive relationship with increasing GHSV while lower hydrocarbon selectivity diminishes.展开更多
Manganese-based cathode materials are considered as a promising candidate for rechargeable aqueous zinc-ion batteries(ZIBs).Suffering from poor conductive and limited structure tolerance,various carbon matrix,especial...Manganese-based cathode materials are considered as a promising candidate for rechargeable aqueous zinc-ion batteries(ZIBs).Suffering from poor conductive and limited structure tolerance,various carbon matrix,especially N-doped carbon,were employed to incorporate with MnO_(2)for greatly promoted electrochemical performances.However,the related underlying mechanism is still unknown,which is unfavorable to guide the design of high performance electrode.Herein,by incorporating layered MnO_(2)with N-doped carbon nanowires,a free-standing cathode with hierarchical core-shell structure(denoted as MnO_(2)@NC)is prepared.Benefiting from the N-doped carbon and rational architecture,the MnO_(2)@NC electrode shows an enhanced specific capacity(325 mAh g^(−1)at 0.1 A g^(−1))and rate performance(90 mAh g^(−1)at 2 A g^(−1)),as well as improved cycling stability.Furthermore,the performance improvement mechanism of MnO_(2)incorporated by N-doped carbon is investigated by X-ray photoelectron spectroscopy(XPS),Raman spectrums and density functional theory(DFT)calculation.The N atom elongates the Mn-O bond and reduces the valence of Mn^(4+)ion in MnO_(2)crystal by delocalizing its electron clouds.Thus,the electrostatic repulsion will be weakened when Zn^(2+)/H^(+)insert into the host MnO_(2)lattices,which is profitable to more cation insertion and faster ion transfer kinetics for higher capacity and rate capability.This work elucidates a fundamental understanding of the functions of N-doped carbon in composite materials and shed light on a practical pathway to optimize other electrode materials.展开更多
Due to the abundance and sustainability of solar energy,converting it into chemical energy to obtain clean energy presents an ideal solution for addressing environmental pollution and energy shortages stemming from th...Due to the abundance and sustainability of solar energy,converting it into chemical energy to obtain clean energy presents an ideal solution for addressing environmental pollution and energy shortages stemming from the extensive combustion of fossil fuels.In recent years,hydrogen energy has emerged on the stage of history as the most promising clean energy carrier of the 21st century.Among the current methods of producing hydrogen,photocatalytic hydrogen production technology,as a zero-carbon approach to producing high calorific value and pollution-free hydrogen energy,has attracted much attention since its discovery.As the core of photocatalysis technology,semiconductor photocatalysts are always the research hotspots.Among them,graphite-phase carbon nitride(g-C_(3)N_(4)),an organic semiconductor material composed of only C and N elements,possesses physicochemical properties incomparable to those of traditional inorganic semiconductor materials,including suitable energy band positions,easy structural regulation,inexpensive raw materials and abundant reserves,simple preparation,high thermal/mechanical/chemical stability,etc.Therefore,g-C_(3)N_(4) has attracted extensive attention in the field of photocatalytic hydrogen production in the last two decades.This review comprehensively outlines the research trajectory of g-C_(3)N_(4) photocatalytic hydrogen production,encompassing development,preparation methods,advantages,and disadvantages.A concise introduction to g-C_(3)N_(4) is provided,as well as an analysis of the underlying mechanism of the photocatalytic system.Additionally,it delves into the latest techniques to enhance performance,including nanostructure design,elemental doping,and heterojunction construction.The applications of g-C_(3)N_(4) based photocatalysts in hydrogen production are surveyed,underscoring the significance of catalyst active sites and g-C_(3)N_(4) synthesis pathways.At length,concluded are insights into the challenges and opportunities presented by g-C_(3)N_(4) based photocatalysts for achieving heightened hydrogen production.展开更多
基金The authors greatly acknowledge the financial support from the National Natural Science Foundation of China(No.51873126)the Fundamental Research Funds for the Central Universities,as well as the funding from the Science&Technology Department(No.2021YFH0123)of Sichuan Province.
文摘Electrically conductive elastomer composites(CECs)with segregated networks of conductive nanofillers show high potential in stretchable strain sensors due to balanced mechanical and electrical properties,yet the sensitivity at low strain is generally insufficient for practical application.Herein,we report an easy and effective way to improve the resistive response to low strain for CECs with segregated network structure via adding stiff alumina into carbon nanostructures(CNS).The CEC containing 0.7 wt%CNS and 5 wt%Al_(2)O_(3) almost sustains the same elasticity(elongation at break of~900%)and conductivity(0.8 S/m)as the control,while the piezoresistive sensitivity is significantly improved.Thermoplastic polyurethane(TPU)composites with a segregated network of hybrid nanofillers(CNS and Al_(2)O_(3))show much higher strain sensitivity(Gauge factor,GF-566)at low strain(45%strain)due to a local stress concentration effect,this sensitivity is superior to that of TPU/CNS composites(GF-11).Such a local stress concentration effect depends on alumina content and its distribution at the TPU particle interface.In addition,CECs with hybrid fillers show better reproducibility in cyclic piezoresistive behavior testing than the control.This work offers an easy method for fabricating CECs with a segregated filler network offering stretchable strain sensors with a high strain sensitivity.
文摘The effect of synthesized nanostructures,including graphene oxide,chemically reduced graphene oxide with sodium dodecyl sulfate(SDS),chemically reduced graphene oxide with polyvinylpyrrolidone,and multi-walled carbon nanotubes,on the kinetics of methane hydrate formation was investigated in this work.The experiments were carried out at a pressure of 4.5 MPa and a temperature of 0 ℃ in a batch reactor.By adding nanostructures,the induction time decreases,and the shortest induction time appeares at certain concentrations of reduced graphene oxide with SDS and graphene oxide,that is,at a concentration of 360 ppm for reduced graphene oxide with SDS and 180 ppm for graphene oxide,with a 98% decrease in induction time compared to that in pure water.Moreover,utilization of carbon nanostructures increases the amount and the rate of methane consumed during the hydrate formation process.Utilization of multi-walled carbon nanotubes with a concentration of 90 ppm showes the highest amount of methane consumption.The amount of methane consumption increases by 173% in comparison with that in pure water.The addition of carbon nanostructures does not change the storage capacity of methane hydrate in the hydrate formation process,while the percentage of water conversion to hydrate in the presence of carbon nanotubes increases considerably,the greatest value of which occurres at a 90 ppm concentration of carbon nanotubes,that is,a 253% increase in the presence of carbon nanotubes compared to that of pure water.
基金financially supported by the National Natural Science Foundation of China (Nos. 21601098 and 51602167)Shandong Provincial Science Foundation (ZR2016EMB07 and ZR2017JL021)+1 种基金Key Research and Development Program (2018GGX102033)Qingdao Applied Fundamental Research Project (16-5-1-92-jch and 17-1-1-81-jch)
文摘A strong interface coupling is of vital importance to develop metal oxide/carbon nanocomposite anodes for next-generation lithium ion batteries.Herein,a rational N-doped carb on riveting strategy is designed to boost the lithium storage performance of Fe3O4/N-doped carbon tubular structures.Poly pyrrole(PPy)has been used as the precursor for N-doped carbon.N-doped carbon-riveted Fe3O4/N-doped carbon(N-C@Fe3O4@N-C)nanocomposites were obtained by pyrolysis of PPy-coated FeOOH@PPy nanotubes in Ar atmosphere.When tested as an anode for LIBs,the N-C@Fe3O4@N-C displays a high reversible discharge capacity of 675.8 mA h g-1 after 100 cycles at a current density of 100 mA g-1 and very good rate capability(470 mA h g_1 at 2 A g-1),which significantly surpasses the performance of Fe3O4@N-C.TEM analysis reveals that after battery cycling the FeOx particles detached from the carbon fibers for Fe3O4@N-C,while for N-C@Fe3O4@N-C the FeOx particles were still trapped in the carbon matrix,thus preserving good electrical contact.Consequently,the superior performance of N-C@Fe3C)4@N-C is attributed to the synergistic effect between Fe3O4 and N-doped carbon combined with the unique structure properties of the nanocomposites.The strategy reported in this work is expected to be applicable for designing other electrode materials for LIBs.
基金financially supported by the National Natural Science Foundation of China(No.51907193 and No.51677182)the Dalian National Laboratory(DNL)for Clean Energy Cooperation Fund,CAS(No.DNL201915 and No.DNL201912)+2 种基金the Beijing Municipal Science and Technology Commission(No.Z181100000118006)the Key Research Program of Frontier Sciences,CAS(No.ZDBS-LY-JSC047)the Youth Innovation Promotion Association,CAS(No.2020000022)。
文摘The burgeoning global economy during the past decades gives rise to the continuous increase in fossil fuels consumption and rapid growth of CO_(2) emission,which demands an urgent exploration into green and sustainable devices for energy storage and power management.Supercapacitors based on activated carbon electrodes are promising systems for highly efficient energy harvesting and power supply,but their promotion is hindered by the moderate energy density compared with batteries.Therefore,scalable conversion of CO_(2) into novel carbon nanostructures offers a powerful alternative to tackle both issues:mitigating the greenhouse effect caused by redundant atmospheric CO_(2) and providing carbon materials with enhanced electrochemical performances.In this tutorial review,the techniques,opportunities and barriers in the design and fabrication of advanced carbon materials using CO_(2) as feedstock as well as their impact on the energy-storage performances of supercapacitors are critically examined.In particular,the chemical aspects of various Cv2 conversion reactions are highlighted to establish a detailed understanding for the science and technology involved in the microstructural evolution,surface engineering and porosity control of CO_(2)-converted carbon nanostructures.Finally,the prospects and challenges associated with the industrialization of CO_(2) conversion and their practical application in supercapacitors are also discussed.
基金supported by the National Natural Science Foundation of China(Grant No.52173091 and 52102300)the Program for Leading Talents of National Ethnic Affairs Commission of China(MZR21001)the Hubei Provincial Natural Science Foundation of China(2021CFA022).
文摘Covalent organic frameworks(COFs)after undergoing the superlithiation process promise high-capacity anodes while suffering from sluggish reaction kinetics and low electrochemical utilization of redox-active sites.Herein,integrating carbon nanotubes(CNTs)with imine-linked covalent organic frameworks(COFs)was rationally executed by in-situ Schiff-base condensation between 1,1′-biphenyl]-3,3′,5,5′-tetracarbaldehyde and 1,4-diaminobenzene in the presence of CNTs to produce core–shell heterostructured composites(CNT@COF).Accordingly,the redox-active shell of COF nanoparticles around one-dimensional conductive CNTs synergistically creates robust three-dimensional hybrid architectures with high specific surface area,thus promoting electron transport and affording abundant active functional groups accessible for electrochemical utilization throughout the whole electrode.Remarkably,upon the full activation with a superlithiation process,the as-fabricated CNT@COF anode achieves a specific capacity of 2324 mAh g^(−1),which is the highest specific capacity among organic electrode materials reported so far.Meanwhile,the superior rate capability and excellent cycling stability are also obtained.The redox reaction mechanisms for the COF moiety were further revealed by Fourier-transform infrared spectroscopy in conjunction with X-ray photoelectron spectroscopy,involving the reversible redox reactions between lithium ions and C=N groups and gradual electrochemical activation of the unsaturated C=C bonds within COFs.
基金Funded by the Innovative Talent Training Project of Chongqing University(CDJXS11220004)the Fundamental Research Funds for the Central Universities of Chongqing University+1 种基金the Natural Science Foundation Project of CQ CSTC(No.2011BB5134)the National Natural Science Foundation of China(No.NSFC81101417)
文摘We previously reported the direct electrochemical detection of insulin at bare carbon electrodes. Here a novel modified acetylene carbon black paste electrode(SiC/CB-CPE), based on the outstanding characteristics of silicon carbide nanostructure,was developed for the electrooxidation of insulin in alkaline solution and it was characterized by cyclic voltammetry(CV) and electrochemical impedance spectroscopy(EIS) in 5 mmol/L Fe(CN)63-/4- solution. It is found that silicon carbide nanostructure doped into the CB-CPE greatly facilitates the redox electrochemistry of Fe(CN)63-/4- probe and the electrochemical oxidation of insulin. The electrooxidation of insulin is a one-electron and one-proton reaction and an irreversible adsorption-controlled electrode process. The anodic oxidation current increases linearly with the concentration of insulin from 1×10-7mol/L to1.2×10-6mol/L in 0.1 mol/L Na2CO3-NaHCO3 buffer solution(pH 10.0) and the detection limit was 50 nmol/L. In addition, the SiC/CB-CPE shows good sensitivity, reproducibility, renewability and capacity of resisting disturbance.
文摘The exploitation of renewable energy as well as the elimination of the harmful impact of excessive carbon emission are worldwide concerns for sustainable development of the ecological environment on earth.To address that,the technologies regarding energy conversion systems,such as water splitting and electroreduction of carbon dioxide,have attracted significant attention for a few decades.Yet,to date,the production of green fuels and/or high energy density chemicals like hydrogen,methane,and ethanol,are still suffering from many drawbacks including high energy consumption,low selectivity,and sluggish reaction rate.In this regard,nanostructured bimetallic materials that is capable of taking the full benefits of the coupling effects between different elements/components with structure modification in nanoscale are considered as a promising strategy for high-performance electrocatalysts.Herein,this review aims to outline the important progress of these nanostructured bimetallic electrocatalysts.It starts with the introduction of some important fundamental background knowledge about the reaction mechanism to understand how these reactions happen.Subsequently,we summarize the most recent progress regarding how the nanostructured bimetallic electrocatalysts manipulate the activity and selectivity of catalytic reactions in the order of bimetallic alloying effect,interface/substrate effect of bi-component electrocatalyst,and nanostructuring effect.
文摘The ability to control the nanoscale shape of carbon nanostructures during wide-scale synthesis process is an essential goal in research for Nanotechnology applications. This paper reports a significant progress toward that goal. Variant CVD has been used for the synthesis of the samples studied. Curvature, hybridization and contamination are analyzed using Electron Microscopies and XANES spectroscopy. The investigations of the results show that four types of samples are obtained. They are carbon nanotubes (CNTs), carbon nanofibers (CNFs), carbon nanowalls (CNWs) and carbon nanoparticles (CNPs). Almost all of them have catalyst nanoparticles (metal) on top in top growth model or on base in base growth model and encapsulated or adsorbed in sidewalls. The orientation of tubular carbon nanomaterials depends on operating parameters. They are classified in three groups: the poorly oriented, the medium oriented and the highly oriented. Their contamination (radicals, atoms and molecules) and hybridization are intrinsically related to the curvature of their graphene layers. XANES spectroscopy allows quantitative characterization of nanomaterials.
文摘An efficient method has been developed to synthesize well-aligned multi-walled carbon nanotubes (MWCNTs) on a conductive Ta substrate by chemical vapour deposition (CVD). Free-standing MWCNTs arrays were functionalized through electrochemical oxidation with the formation of hydroxyl and carboxyl functional groups. Using a new oven drying technique, we demonstrate that the unidirectionally aligned and laterally spaced geometry of the CNT arrays can be retained after being subjected to each step of electrochemical modification. Samples were analyzed by using a field emission scanning electron microscope (SEM), transmission electron microscope (TEM), Fourier transformed infrared (FTIR) and Raman spectroscopy. Useful electrochemical methods for the synthesis of various gold nanostructures onto the aligned MWCNTs were then presented for the first time. The results demonstrated that flowerlike nanoparticle arrays, nanosheets and nanoflowers were obtained on the aligned CNTs under different experimental conditions. These kinds of aligned-CNT/Au nanostructures hybrid materials introduced by these efficient and simple electrochemical methods could lead to development of a new generation device for ultrasensitive catalytic and biological application.
文摘Natural rubber based composites containing different carbon nanofillers (fullerenes, carbon nanotubes (CNTs) and graphene nanoplatelets (GNPs)) at different concentrations have been prepared. Their dielectric properties (dielectric permittivity, dielectric loss) have been studied in the 1 - 12 GHz frequency range. Some factors (electromagnetic field frequency, fillers concentration, fillers intrinsic structure) influencing the dielectric behavior of the composites have been investigated. The dielectric properties of the developed natural rubber composites containing conductive fillers (fullerenes, CNTs, GNPs) indicate that these composites can be used as broadband microwave absorbing materials.
文摘X-Ray Absorption Spectroscopy (XAS) on the carbon K edge of carbon nanostructures (nanotubes, nanofibers, nanowalls) is reported here. They are grown on plain SiO2 (8 nm thick)/Si(100) substrates by a Plasma and Hot Filaments-enhanced Catalytic Chemical Vapor Deposition (PE HF CCVD) process. The morphology and the nature of these carbon nanostructures are characterized by SEM, TEM and Raman spectroscopy. According to conditions of catalyst preparation and DC HF CCVD process, carbon nanotubes (CNTs), carbon nanofibers (CNFs), carbon nanowalls (CNWs), carbon nanoparticles (CNPs) with different orientation of the graphene plans or shells can be prepared. From the angular dependence of the incident light and geometrical morphology of the nanostructures, wide variations of the C K-edge intensity of the transitions to the empty π* and σ* states occur. A full lineshape analysis of the XAS spectra has been carried out using a home-made software, allowing estimating the relative proportion of π* and σ* transitions. A geometrical model of the angular dependence with the incidence angle of the light and the morphology of the carbon nanostructures is derived. With normalization to the HOPG (Highly Oriented Pyrolytic Graphite graphite) reference case, a degree of alignment can be extracted which is representative of the localized orientation of the graphitic carbon π bonds, accounting not only for the overall orientation, but also for local defects like impurities incorporation, structural defects ... This degree of alignment shows good agreement with SEM observations. Thus CNTs films display degrees of alignment around 50%, depending on the occurrence of defects in the course of the growth, whereas no special alignment can be detected with CNFs and CNPs, and a weak one (about 20%) is detected on CNWs.
基金supported by the National Natural Science Foundation of China(22179063)。
文摘VS_(4) has a unique layered atomic chain structure and has the potential to become a high-performance cathode material of magnesium-ion batteries with a high capacity and long cycle life.However,low conductivity and sluggish Mg^(2+)diffusivity during cycling limit its practical application in large-scale energy storage.Herein,a cooperative assembly-directed strategy is adopted to synthesize VS_(4) nanorods grown in situ on carbon nanotubes(CNTs/VS_(4)).VS_(4) nanorods are tightly anchored to CNTs through V-O-C interface covalent bonds,and CNTs can enhance the electronic conductivity of the nanocomposite.In addition,the ion insertion reaction using Mg^(2+)and Mg Cl^(+)as carriers reduces the polar barrier for divalent Mg^(2+)ion transport.This rationally designed architecture promotes ion diffusion and electron transfer,thus facilitating reaction kinetics.The cooperative assembly-oriented strategy can endow CNTs/VS_(4) with excellent magnesium storage properties,including a high reversible capacity of 223.2 m Ah g^(-1)at a current density of 50 m A g^(-1),a remarkable discharge capacity of 91.8 m Ah g^(-1)even at 2,000 m A g^(-1),and an impressive capacity retention of 85.2% after 1,000 cycles at 500 m A g^(-1).Moreover,this strategy can serve as a general synthetic method for the complexation of VS_(4) with other carbon nanostructures.
基金supported by the Iran National Science Foundation (INSF) under the contract number 87040961the Iranian Nano Technology Initiative Council
文摘An extensive study of Fischer-Tropsch synthesis on nanostructure supports with high surface area such as nanostructure -y-alumina, single wall carbon nanotubes (SWNTs), and the hybrid of SWNTs/nanostructure -y-alumina has been investigated. The nanostructure γ-alumina was promoted with lanthanum to obtain better performance of catalyst and 15 wt% cobalt loading was the basis of our investigation. Fischer- Tropsch synthesis was performed in a fixed bed reactor under different reaction conditions (220-240 ℃, 15-25 bar, H2/CO ratio of 2, GHSV of 900-1400) in order to study the effects of temperature, pressure and gas hourly space velocity (GHSV) changes on hydrocarbon selec- tivity and catalyst activity. The catalysts were extensively characterized by different methods including X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), inductively coupled plasma (ICP), hydrogen (H2) chemisorption and temperature-programmed reduction (TPR). The results showed that the yield of hybrid supported catalyst (55.4%) is higher than that of nanos- tructure -y-alumina supported catalyst (55.0%) and lower than that of SWNTs supported cobalt catalyst (71.0%). The hybrid supported catalyst showed higher reduction degree and dispersion of cobalt particles. The temperature, pressure and GHSV effects on hybrid supported catalyst were studied and results showed that higher pressure favors the chain growth and temperature increase leads to the increases in methane selec- tivity and CO conversion. Higher hydrocarbon selectivity and CO conversion showed positive relationship with increasing GHSV while lower hydrocarbon selectivity diminishes.
基金supported by National Natural Science Foundation of China(Nos.U20A20246,51872108)the Fundamental Research Funds for the Central Universities(Nos.30106200463 and CCNU20TS006)Graduate Education Innovation Grant from Central China Normal University(No.2020CXZZ101).
文摘Manganese-based cathode materials are considered as a promising candidate for rechargeable aqueous zinc-ion batteries(ZIBs).Suffering from poor conductive and limited structure tolerance,various carbon matrix,especially N-doped carbon,were employed to incorporate with MnO_(2)for greatly promoted electrochemical performances.However,the related underlying mechanism is still unknown,which is unfavorable to guide the design of high performance electrode.Herein,by incorporating layered MnO_(2)with N-doped carbon nanowires,a free-standing cathode with hierarchical core-shell structure(denoted as MnO_(2)@NC)is prepared.Benefiting from the N-doped carbon and rational architecture,the MnO_(2)@NC electrode shows an enhanced specific capacity(325 mAh g^(−1)at 0.1 A g^(−1))and rate performance(90 mAh g^(−1)at 2 A g^(−1)),as well as improved cycling stability.Furthermore,the performance improvement mechanism of MnO_(2)incorporated by N-doped carbon is investigated by X-ray photoelectron spectroscopy(XPS),Raman spectrums and density functional theory(DFT)calculation.The N atom elongates the Mn-O bond and reduces the valence of Mn^(4+)ion in MnO_(2)crystal by delocalizing its electron clouds.Thus,the electrostatic repulsion will be weakened when Zn^(2+)/H^(+)insert into the host MnO_(2)lattices,which is profitable to more cation insertion and faster ion transfer kinetics for higher capacity and rate capability.This work elucidates a fundamental understanding of the functions of N-doped carbon in composite materials and shed light on a practical pathway to optimize other electrode materials.
基金supported by the National Natural Science Foundation of China(22202086,22208129)Postgraduate Research&Practice Innovation Program of Jiangsu Province(SJCX23_2070)College Student Innovation and Practice Fund of Industrial Center of Jiangsu University(ZXJG2022002).
文摘Due to the abundance and sustainability of solar energy,converting it into chemical energy to obtain clean energy presents an ideal solution for addressing environmental pollution and energy shortages stemming from the extensive combustion of fossil fuels.In recent years,hydrogen energy has emerged on the stage of history as the most promising clean energy carrier of the 21st century.Among the current methods of producing hydrogen,photocatalytic hydrogen production technology,as a zero-carbon approach to producing high calorific value and pollution-free hydrogen energy,has attracted much attention since its discovery.As the core of photocatalysis technology,semiconductor photocatalysts are always the research hotspots.Among them,graphite-phase carbon nitride(g-C_(3)N_(4)),an organic semiconductor material composed of only C and N elements,possesses physicochemical properties incomparable to those of traditional inorganic semiconductor materials,including suitable energy band positions,easy structural regulation,inexpensive raw materials and abundant reserves,simple preparation,high thermal/mechanical/chemical stability,etc.Therefore,g-C_(3)N_(4) has attracted extensive attention in the field of photocatalytic hydrogen production in the last two decades.This review comprehensively outlines the research trajectory of g-C_(3)N_(4) photocatalytic hydrogen production,encompassing development,preparation methods,advantages,and disadvantages.A concise introduction to g-C_(3)N_(4) is provided,as well as an analysis of the underlying mechanism of the photocatalytic system.Additionally,it delves into the latest techniques to enhance performance,including nanostructure design,elemental doping,and heterojunction construction.The applications of g-C_(3)N_(4) based photocatalysts in hydrogen production are surveyed,underscoring the significance of catalyst active sites and g-C_(3)N_(4) synthesis pathways.At length,concluded are insights into the challenges and opportunities presented by g-C_(3)N_(4) based photocatalysts for achieving heightened hydrogen production.
基金the National Natural Science Foundation of China(Nos.51271035 and 51371032)for funding this workfinancial support from the National Natural Science Foundation of China(No.51204092)the Key Laboratory Fundamental Research Project of the Education Department of Liaoning Province,China(No.LZ2015046)