Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing...Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing performance.However,previous methods of synthesizing MO_(x)/C composites suffer from problems,including inhomogeneity,aggregation,and challenges in micropatterning.Herein,we introduce a refined method that employs a metal–organic framework(MOF)as a precursor combined with direct laser writing.The inherent structure of MOFs ensures a uniform distribution of metal ions and organic linkers,yielding homogeneous MO_(x)/C structures.The laser processing facilitates precise micropatterning(<2μm,comparable to typical photolithography)of the MO_(x)/C crystals.The optimized MOF-derived MO_(x)/C sensor rapidly detected ethanol gas even at room temperature(105 and 18 s for response and recovery,respectively),with a broad range of sensing performance from 170 to 3,400 ppm and a high response value of up to 3,500%.Additionally,this sensor exhibited enhanced stability and thermal resilience compared to previous MOF-based counterparts.This research opens up promising avenues for practical applications in MOF-derived sensing devices.展开更多
Organic-inorganic MoO_(3)/PI(MoPI)composites were prepared using a simple one-pot thermal copolymerization method.The resulting composites exhibited enhanced photocatalytic activity for the selective oxidation of benz...Organic-inorganic MoO_(3)/PI(MoPI)composites were prepared using a simple one-pot thermal copolymerization method.The resulting composites exhibited enhanced photocatalytic activity for the selective oxidation of benzylamine to N-benzylidene benzylamine(N-BDBA)in ambient air under simulated solar light irradiation compared to pristine MoO_(3) or polyimide(PI).In particular,the MoPI composite with a 0.3:1 molar ratio of Mo to melamine,referred to as MoPI-0.3,demonstrated the best performance in the photo-oxidation of benzylamine,achieving a benzylamine conversion of 95%with a N-BDBA selectivity exceeding 99%after 3 h irradiation.The enhanced photocatalytic activity of the MoPI-0.3 catalyst was attributed to the formation of a direct Z-scheme heterojunction between MoO_(3) and PI,facilitating more efficient separation of the photoinduced electrons and holes.Additionally,the MoPI-0.3 composite maintained considerably high activity over four consecutive cycles,highlighting its good stability and recyclability.Furthermore,the MoPI-0.3 composite could photo-oxidize benzylamine derivatives and heterocyclic amines to their corresponding imines,demonstrating the universal applicability of this composite catalyst.展开更多
Cu-Fe composite oxides were prepared by co-precipitation method and tested for higher alcohol synthesis from syngas. The selectivity to C2＋OH and C6＋OH in alcohol distribution was very high while the methane product...Cu-Fe composite oxides were prepared by co-precipitation method and tested for higher alcohol synthesis from syngas. The selectivity to C2＋OH and C6＋OH in alcohol distribution was very high while the methane product fraction in hydrocarbon distribution was rather low, demonstrating a promising potential in higher alcohols synthesis from syngas. The distribution of alcohols and hydrocarbons approximately obeyed Anderson-Schulz-Flory distribution with similar chain growth probability, indicating alcohols and hydrocarbons derived from the same intermediates. The effects of Cu/Fe molar ratio, reaction temperature and gas hourly space velocity （GHSV） on catalytic performance were studied in detail. The sample with a Cu/Fe molar ratio of 10/1 exhibited the best catalytic performance. Higher reaction temperature accelerated water-gas-shift reaction and led to lower total alcohols selectivity. GHSV showed great effect on catalytic performance and higher GHSV increased the total alcohol selectivity, indicating there existed visible dehydration reaction of alcohol into hydrocarbon.展开更多
In this study, coral?like yolk–shell?structured NiO/C composite microspheres(denoted as CYS?NiO/C) were prepared using spray pyrolysis. The unique yolk–shell structure was characterized, and the formation mechanism ...In this study, coral?like yolk–shell?structured NiO/C composite microspheres(denoted as CYS?NiO/C) were prepared using spray pyrolysis. The unique yolk–shell structure was characterized, and the formation mechanism of the structure was proposed. Both the phase separation of the polyvinylpyrrolidone and polystyrene(PS) colloidal solution and the decompo?sition of the size?controlled PS nanobeads in the droplet played crucial roles in the formation of the unique coral?like yolk–shell structure. The CYS?NiO/C microspheres delivered a reversible discharge capacity of 991 mAh g^(-1) after 500 cycles at the current density of 1.0 A g^(-1). The dis?charge capacity of the CYS?NiO/C microspheres after the 1000 th cycle at the current density of 2.0 A g^(-1) was 635 mAh g^(-1), and the capacity retention measured from the second cycle was 91%. The final discharge capacities of the CYS?NiO/C microspheres at the current densities of 0.5, 1.5, 3.0, 5.0, 7.0, and 10.0 A g^(-1) were 753, 648, 560, 490, 440, and 389 mAh g^(-1), respectively. The synergetic e ect of the coral?like yolk–shell structure with well?defined interconnected mesopores and highly conductive carbon resulted in the excellent Li+?ion storage properties of the CYS?NiO/C microspheres.展开更多
The electrical and optical properties of the indium tin oxide （ITO）/epoxy composite exhibit dramatic variations as functions of the ITO composition and ITO particle size. Sharp increases in the conductivity in the v...The electrical and optical properties of the indium tin oxide （ITO）/epoxy composite exhibit dramatic variations as functions of the ITO composition and ITO particle size. Sharp increases in the conductivity in the vicinity of a critical volume fraction have been found within the framework of percolation theory. A conductive and insulating transition model is extracted by the ITO particle network in the SEM image, and verified by the resistivity dependence on the temperature. The dependence of the optical transmittance on the particle size was studied. Further decreasing the ITO particle size could further improve the percolation threshold and light transparency of the composite film.展开更多
Ceria-based heterostructure composite(CHC)has become a new stream to develop advanced low-temperature(300–600°C)solid oxide fuel cells(LTSOFCs)with excellent power outputs at 1000 mW cm−2 level.The state-ofthe-a...Ceria-based heterostructure composite(CHC)has become a new stream to develop advanced low-temperature(300–600°C)solid oxide fuel cells(LTSOFCs)with excellent power outputs at 1000 mW cm−2 level.The state-ofthe-art ceria–carbonate or ceria–semiconductor heterostructure composites have made the CHC systems significantly contribute to both fundamental and applied science researches of LTSOFCs;however,a deep scientific understanding to achieve excellent fuel cell performance and high superionic conduction is still missing,which may hinder its wide application and commercialization.This review aims to establish a new fundamental strategy for superionic conduction of the CHC materials and relevant LTSOFCs.This involves energy band and built-in-field assisting superionic conduction,highlighting coupling effect among the ionic transfer,band structure and alignment impact.Furthermore,theories of ceria–carbonate,e.g.,space charge and multi-ion conduction,as well as new scientific understanding are discussed and presented for functional CHC materials.展开更多
Poly(decamethylene terephthalamide/decamethylene isophthalamide)-block-polyvinyl alcoho)(PA10 T/10 IPEG) copolymer/graphene oxide(GO) composites were prepared via in-situ melt polymerization and two different nano-fil...Poly(decamethylene terephthalamide/decamethylene isophthalamide)-block-polyvinyl alcoho)(PA10 T/10 IPEG) copolymer/graphene oxide(GO) composites were prepared via in-situ melt polymerization and two different nano-filler addition approaches were compared. The relationship between the micro-structure and performance of the elastomer composites prepared by one-step and two-step methods was explored. The results show that the two-step method significantly promoted the dispersion of the GO in a polymer matrix, and facilitated the grafting of more hard molecular chains. Thus, the elastic modulus and tensile strength of the nanocomposite have been significantly improved by the presence of GO. This was because of the strong interaction between the functional groups on the surface of the GO and the hard molecular chains. This would be also be favorable to load transfer across the interface. Additionally, the elongation at the break of composites increased by 10% with the addition of a small amount of GO(0.2% wt). This is because hard domains tend to be enriched on the surface of GO in composites and act as a lubricating layer at the interface between the GO and matrix, leading to increased deformation ability. This work provides an effective strategy to prepare elastomer composites with high strength and toughness.展开更多
A series of novel Ni/CeOe-Al2O3 composite catalysts were synthesized by one-step citric acid complex method, The as-synthesized catalysts were characterized by N2 physical adsorption/desorption, X-ray diffraction （XR...A series of novel Ni/CeOe-Al2O3 composite catalysts were synthesized by one-step citric acid complex method, The as-synthesized catalysts were characterized by N2 physical adsorption/desorption, X-ray diffraction （XRD）, Fourier transform infrared （FT-IR） spectroscopy, hydrogen temperature-programmed reduction （Hz-TPR）, X-ray photoelectron spectroscopy （XPS） and thermogravimetry analysis （TGA）. The effects of nickel content, calcination and reaction temperatures, gas hourly space velocity （GHSV） and inert gas dilution of N2 on their performance of catalytic partial oxidation of methane （CPOM） were investigated. Catalytic activity test results show that the highest methane conversion （〉85%）, the best selectivities to carbon monoxide （〉87%） and to hydrogen （〉95%）, the excellent stability and perfect Hz/CO ratio （2.0） can be obtained over Ni/CeO2-Al2O3 with 8 wt% Ni content calcined at 700 ℃ under the reaction condition of 750 ℃, CH4/O2 ratio of 2 ： 1 and gas hourly space velocity of 12000 mL.h-1 .g-1. Characterization results show that the good catalytic performance of this composite catalyst can be contributed to its large specific surface area （~108 m2.g-1）, small crystallite size, easy reducibility and low coking rate.展开更多
The experimental values of the enthalpy of formation of two isomeric 3,4-and 3,5-dinitro-1-(trinitromethyl)-1H-pyrazoles have been obtained(261.5±5.0and 246.4±6.7kJ/mol for crystalline 3,4-and 3,5-dinitro-1-...The experimental values of the enthalpy of formation of two isomeric 3,4-and 3,5-dinitro-1-(trinitromethyl)-1H-pyrazoles have been obtained(261.5±5.0and 246.4±6.7kJ/mol for crystalline 3,4-and 3,5-dinitro-1-(trinitromethyl)-1H-pyrazoles,respectively).The ballistic effectiveness of these potential oxidizers in composite solid propellants was studied.It is shown that these two oxidizers may be successfully applied in metal-free compositions or with a small content of metal.For the bottom stage 3,4-dinitro-1-(trinitromethyl)-1H-pyrazole is a bit better than 3,5-dinitro-1-(trinitromethyl)-1H-pyrazole,for the upper stage the both oxidizers show the equal ballistic parameters.These oxidizers allow to create metal-free solid composite propellants with the binder percentage not lower than 19%(volume fraction),with I3spequal to 256.5-257.0sat density equal to 1.72-1.74g/cm^3.展开更多
Ti_(0.2)Zr_(0.2)Hf_(0.2)Nb_(0.2)Ta_(0.2)C-M_(t)C composite ceramic was prepared by hot press sintering,with the Ti_(0.2)Zr_(0.2)Hf_(0.2)Nb_(0.2)Ta_(0.2)C high-entropy carbide as the main phase.Secondary phase M_(x)C(M...Ti_(0.2)Zr_(0.2)Hf_(0.2)Nb_(0.2)Ta_(0.2)C-M_(t)C composite ceramic was prepared by hot press sintering,with the Ti_(0.2)Zr_(0.2)Hf_(0.2)Nb_(0.2)Ta_(0.2)C high-entropy carbide as the main phase.Secondary phase M_(x)C(M=Ti,Zr,Hf,Nb,Ta) was found to be distributed relatively uniform in the composite ceramic.The oxidation behavior of the ceramic was examined after exposure to 923 K and 1173 K.Morphology of the surface and cross sections of all oxidation samples were observed.The characteristics of the oxidation behavior of the high-entropy carbide and the secondary phase M_(x)C were compared and analyzed.The secondary phases(such as Ti-rich carbide or Hf-rich carbide) in the material were seriously oxidized at 923 K and 1173 K,which reflects the superior oxidation performance of the high-entropy carbide.The nano high-entropy oxides with Ti,Zr,Hf,Nb,Ta,and O elements were discovered by oxidation of the composite ceramic.This research will help deepen the understanding of the oxidation mechanism of high-entropy carbide and composite ceramic.展开更多
Bulk Ni-Mo composites were prepared by a simple solid reaction method and the hydrodeoxygenation activity of samples was examined. The test results showed that the Ni-Mo catalysts possessed high catalytic activity for...Bulk Ni-Mo composites were prepared by a simple solid reaction method and the hydrodeoxygenation activity of samples was examined. The test results showed that the Ni-Mo catalysts possessed high catalytic activity for hydrogenation of p-cresol under mild conditions. The XRD, N_2 isothermal adsorption, NH_3-TPD characterization analyses indicated that the excellent hydrogenation performance of Ni-Mo catalysts could be attributed to their incorporated Mo metal, the developed pore system, and the strong acidity.展开更多
Titanium oxide films were prepared by annealing DC magnetron sputtered titanium films in an oxygen ambient. X-ray diffraction （XRD）, Auger electron spectroscopy （AES） sputter profiling, MCs^＋-mode secondary ion m...Titanium oxide films were prepared by annealing DC magnetron sputtered titanium films in an oxygen ambient. X-ray diffraction （XRD）, Auger electron spectroscopy （AES） sputter profiling, MCs^＋-mode secondary ion mass spectrometry （MCs^＋-SIMS） and atomic force microscopy （AFM） were employed, respectively, for the structural, com- positional and morphological characterization of the obtained films. For temperatures below 875 K, titanium films could not be fully oxidized within one hour. Above that temperature, the completely oxidized films were found to be rutile in structure. Detailed studies on the oxidation process at 925K were carried out for the understanding of the underlying mechanism of titanium dioxide （TiO2） formation by thermal oxidation. It was demonstrated that the formation of crystalline TiO2 could be divided into a short oxidation stage, followed by crystal forming stage. Relevance of this recognition was further discussed.展开更多
Carbon nanotubes-Nafion （CNTs-Nation） composites were prepared by impregnated CNTs with Nation in ethanol solution and characterized by FT-IR. Pt-Ru catalysts supported on CNTs-Nafion composites were synthesized by ...Carbon nanotubes-Nafion （CNTs-Nation） composites were prepared by impregnated CNTs with Nation in ethanol solution and characterized by FT-IR. Pt-Ru catalysts supported on CNTs-Nafion composites were synthesized by microwave-assisted polyol process. The physical and electrochemical properties of the catalysts were characterized by X-ray diffraction （XRD）, transmission electron microscope （TEM）, CO stripping voltammetry, cyclic voltammetry （CV） and chronoamperometry （CA）. The results showed that the Nation incorporation in CNTs-Nation composites did not significantly alter the oxygen-containing groups on the CNTs surface. The Pt-Ru catalyst supported on CNTs-Nafion composites with 2 wt% Naton showed good dispersion and the best CO oxidation and methanol electro-oxidation activities.展开更多
Exploiting high-efficiency Ni-based materials for electrocatalytic urea oxidation reaction(UOR) is critical for urea-related technologies.The catalytic site density,intrinsic activity,charge transfer,and mass diffusio...Exploiting high-efficiency Ni-based materials for electrocatalytic urea oxidation reaction(UOR) is critical for urea-related technologies.The catalytic site density,intrinsic activity,charge transfer,and mass diffusion determine overall electrocatalytic efficiency.Simultaneous modulation over the above four factors promises advanced electrocatalysis,yet challenging.Herein we propose a systematic regulation tactic over composition and geometric structure,constructing a nanocomposite comprising Mn doped Ni_(3)N nanoparticles anchored on reduced graphene oxide(rGO/Mn-Ni_(3)N),achieving elegant integration of four design principles into one,thereby eminently boosting UOR.Particularly,Mn doping in Ni_(3)N can modulate electronic state to induce intrinsic activity regulation.Combining metallic Mn-Ni_(3)N with rGO to engineer hierarchical architecture not only promotes charge transfer,but also enriches active site population.Intriguingly,improved hydrophilicity could impart better electrolyte penetration and gas escape.Consequently,such system-optimized rGO/Mn-Ni_(3)N demonstrates state-of-the-art-level UOR electrocatalysis.This work offers a novel paradigm to create advanced catalysts via systematic and integrated modulation.展开更多
High activity and productivity of MoVNbTeO_(x) catalyst are challenging tasks in oxidative dehydrogenation of ethane(ODHE)for industrial application.In this work,phase-pure M1 with 30 wt%CeO_(2) composite catalyst was...High activity and productivity of MoVNbTeO_(x) catalyst are challenging tasks in oxidative dehydrogenation of ethane(ODHE)for industrial application.In this work,phase-pure M1 with 30 wt%CeO_(2) composite catalyst was treated by oxygen plasma to further enhance catalyst performance.The results show that the oxygen vacancies generated by the solid-state redox reaction between M1 and CeO_(2) capture active oxygen species in gas and transform V^(4+)to V^(5+)without damage to M1 structure.The space-time yield of ethylene of the plasma-treated catalyst was significantly increased,in which the catalyst shows an enhancement near~100% than that of phase-pure M1 at 400℃ for ODHE process.Plasma treatment for catalysts demonstrates an effective way to convert electrical energy into chemical energy in catalyst materials.Energy conversion is achieved by using the catalyst as a medium.展开更多
In this study,we successfully synthesized double perovskite-type oxide NdBa0.5Ca0.5Co1.5Fe0.5O5+δ(NBCCF)using a conventional wet chemical method as the oxygen electrode for reversible solid oxide electrochemical cell...In this study,we successfully synthesized double perovskite-type oxide NdBa0.5Ca0.5Co1.5Fe0.5O5+δ(NBCCF)using a conventional wet chemical method as the oxygen electrode for reversible solid oxide electrochemical cells(RSOCs).The polarization resistance(Rp)of the composite electrode NBCCFGd0.1Ce0.9O2(GDC)is only 0.079Ωcm^2 at 800℃under air.The single cell based on NBCCF-GDC electrode displays a peak power density of 0.941 W/cm^2 in fuel cell mode and a low Rp value of 0.134Ωcm^2.In electrolysis cell mode,the cell displays an outstanding oxygen evolution reaction(OER)activity and shows current density as high as 0.92 A/cm^2 with 50 vol%AH(Absolute Humidity)at 800℃and applied voltage of 1.3 V.Most importantly,the cell exhibits admirable durability of 60 h both in electrolysis mode and fuel cell mode with distinguished reversibility.All these results suggest that NBCCF is a promising candidate electrode for RSOC.展开更多
The high-energy lithium/sulfur(Li/S) battery has become a very popular topic of research in recent years due to its high theoretical capacity of 1672 m Ah/g. However, the polysulfide shuttle effect remains of great co...The high-energy lithium/sulfur(Li/S) battery has become a very popular topic of research in recent years due to its high theoretical capacity of 1672 m Ah/g. However, the polysulfide shuttle effect remains of great concern with a great number of publications dedicated to its mitigation. In this contribution, a three-dimensional(3D) reduced graphene oxide/activated carbon(RGO/AC) film, synthesized by a simple hydrothermal method and convenient mechanical pressing, is sandwiched between the separator and the sulfur-based cathode, acting as a functional interlayer to capture and trap polysulfide species. Consequently, the Li/S cell with this interlayer shows an impressive initial discharge capacity of 1078 m Ah/g and a reversible capacity of 655 m Ah/g even after 100 cycles. The RGO/AC interlayer impedes the movement of polysulfide while providing unimpeded channels for lithium ion mass transfer. Therefore, the RGO/AC interlayer with a well-designed structure represents strong potential for high-performance Li/S batteries.展开更多
This article reported the electrochemical behaviors of a novel hollow carbon microspheres/manganese dioxide nanosheets(micro-HC/nano-MnO2) composite prepared by an in situ self-limiting deposition method under hydroth...This article reported the electrochemical behaviors of a novel hollow carbon microspheres/manganese dioxide nanosheets(micro-HC/nano-MnO2) composite prepared by an in situ self-limiting deposition method under hydrothermal condition. The results of scanning electron microscopy reveal that MnO2 nanosheets homogeneously grow onto the surface of micro-HC to form a loose-packed microstructure. The quantity of MnO2 required in the electrode layer has thereby been reduced significantly, and higher specific capacitances have been achieved. The micro-HC/nano-MnO2 electrode presents a high capacitance of 239.0 F g-1 at a current density of 5 m A cm-2, which is a strong promise for high-rate electrochemical capacitive energy storage applications.展开更多
Natural intercalation of the graphite oxide, obtained as a product of Hummer＇s method, via ultra-sonication of water dispersed graphite oxide has been carried out to obtain graphene oxide（GO） and thermally reduced ...Natural intercalation of the graphite oxide, obtained as a product of Hummer＇s method, via ultra-sonication of water dispersed graphite oxide has been carried out to obtain graphene oxide（GO） and thermally reduced graphene oxide（RGO）.Here we report the effect of metallic nitrate on the oxidation properties of graphite and then formation of metallic oxide（MO） composites with GO and RGO for the first time. We observed a change in the efficiency of the oxidation process as we replaced the conventionally used sodium nitrate with that of nickel nitrate Ni（NO_3）_2, cadmium nitrate Cd（NO_3）_2,and zinc nitrate Zn（NO_3）_2. The structural properties were investigated by x-ray diffraction and observed the successful formation of composite of MO–GO and MO–RGO（M = Zn, Cd, Ni）. We sought to study the effect on the oxidation process through optical characterization via UV-Vis spectroscopy and Fourier Transform Infrared（FTIR） spectroscopy.Moreover, Thermo Gravimetric Analysis（TGA） was carried out to confirm 〉 90% weight loss in each process thus proving the reliability of the oxidation cycles. We have found that the nature of the oxidation process of graphite powder and its optical and electrochemical characteristics can be tuned by replacing the sodium nitrate（NaNO_3） by other metallic nitrates as Cd（NO_3）_2, Ni（NO_3）_2, and Zn（NO_3）_2. On the basis of obtained results, the synthesized GO and RGO may be expected as a promising material in antibacterial activity and in electrodes fabrication for energy devices such as solar cell, fuel cell,and super capacitors.展开更多
The emergency of high-power electrical appliances has put forward higher requirements for the power density of lithium-ion batteries.Vanadium oxides with large theoretical capacities and high operating voltages are co...The emergency of high-power electrical appliances has put forward higher requirements for the power density of lithium-ion batteries.Vanadium oxides with large theoretical capacities and high operating voltages are considered as prospective alternatives for the cathode of a new generation of lithium-ion batteries.However,the poor rate and cycling performance caused by the sluggish electrons/lithium transportation,irreversible phase changes,vanadium dissolution and large volume changes during the repeated lithium intercalation/deintercalation hinder their commercial development.Several optimizing routes have been carried out and extensively explored to address these problems.Taking V_(2)O_(5),VO_(2)(B),V_(6)O_(13),and V_(2)O_(3)as examples,this article reviewed their crystal structures and lithium storage reactions.Besides,recent progress in modification methods for the electrochemical insufficiencies of vanadium oxides,including nanostructure,heterogeneous atom doping,composite and self-supported electrodes has been systematically summarized and finally,the challenges for the industrialization of vanadium oxide cathodes and their development opportunities are proposed.展开更多
基金supported by the National Research Foundation of Korea(NRF)grants funded by the Ministry of Science and ICT(MSIT)(RS-2023-00251283,and 2022M3D1A2083618)by the Ministry of Education(2020R1A6A1A03040516).
文摘Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing performance.However,previous methods of synthesizing MO_(x)/C composites suffer from problems,including inhomogeneity,aggregation,and challenges in micropatterning.Herein,we introduce a refined method that employs a metal–organic framework(MOF)as a precursor combined with direct laser writing.The inherent structure of MOFs ensures a uniform distribution of metal ions and organic linkers,yielding homogeneous MO_(x)/C structures.The laser processing facilitates precise micropatterning(<2μm,comparable to typical photolithography)of the MO_(x)/C crystals.The optimized MOF-derived MO_(x)/C sensor rapidly detected ethanol gas even at room temperature(105 and 18 s for response and recovery,respectively),with a broad range of sensing performance from 170 to 3,400 ppm and a high response value of up to 3,500%.Additionally,this sensor exhibited enhanced stability and thermal resilience compared to previous MOF-based counterparts.This research opens up promising avenues for practical applications in MOF-derived sensing devices.
基金supported by the Opening Project of Key Laboratory of Green Catalysis of Higher Education Institutes of Sichuan (LZJ2101)the Fundamental Research Funds of China West Normal University (19D038)
文摘Organic-inorganic MoO_(3)/PI(MoPI)composites were prepared using a simple one-pot thermal copolymerization method.The resulting composites exhibited enhanced photocatalytic activity for the selective oxidation of benzylamine to N-benzylidene benzylamine(N-BDBA)in ambient air under simulated solar light irradiation compared to pristine MoO_(3) or polyimide(PI).In particular,the MoPI composite with a 0.3:1 molar ratio of Mo to melamine,referred to as MoPI-0.3,demonstrated the best performance in the photo-oxidation of benzylamine,achieving a benzylamine conversion of 95%with a N-BDBA selectivity exceeding 99%after 3 h irradiation.The enhanced photocatalytic activity of the MoPI-0.3 catalyst was attributed to the formation of a direct Z-scheme heterojunction between MoO_(3) and PI,facilitating more efficient separation of the photoinduced electrons and holes.Additionally,the MoPI-0.3 composite maintained considerably high activity over four consecutive cycles,highlighting its good stability and recyclability.Furthermore,the MoPI-0.3 composite could photo-oxidize benzylamine derivatives and heterocyclic amines to their corresponding imines,demonstrating the universal applicability of this composite catalyst.
基金the State Key Fundamental Research Program(Ministry of Science and Technology of China,No.2011CBA00501)Shanghai Municipal Science and Technology Commission,China(Grant No:11DZ1200300)the Foundation of State Key Laboratory of Coal Conversion(Grant No:1112610)
文摘Cu-Fe composite oxides were prepared by co-precipitation method and tested for higher alcohol synthesis from syngas. The selectivity to C2＋OH and C6＋OH in alcohol distribution was very high while the methane product fraction in hydrocarbon distribution was rather low, demonstrating a promising potential in higher alcohols synthesis from syngas. The distribution of alcohols and hydrocarbons approximately obeyed Anderson-Schulz-Flory distribution with similar chain growth probability, indicating alcohols and hydrocarbons derived from the same intermediates. The effects of Cu/Fe molar ratio, reaction temperature and gas hourly space velocity （GHSV） on catalytic performance were studied in detail. The sample with a Cu/Fe molar ratio of 10/1 exhibited the best catalytic performance. Higher reaction temperature accelerated water-gas-shift reaction and led to lower total alcohols selectivity. GHSV showed great effect on catalytic performance and higher GHSV increased the total alcohol selectivity, indicating there existed visible dehydration reaction of alcohol into hydrocarbon.
基金supported by the National Research Foundation of Korea (NRF) Grant funded by the Korea government (MSIP) (NRF-2018R1A4A1024691, NRF-2017M1A2A2087577, and NRF-2018R1D1A3B07042514)
文摘In this study, coral?like yolk–shell?structured NiO/C composite microspheres(denoted as CYS?NiO/C) were prepared using spray pyrolysis. The unique yolk–shell structure was characterized, and the formation mechanism of the structure was proposed. Both the phase separation of the polyvinylpyrrolidone and polystyrene(PS) colloidal solution and the decompo?sition of the size?controlled PS nanobeads in the droplet played crucial roles in the formation of the unique coral?like yolk–shell structure. The CYS?NiO/C microspheres delivered a reversible discharge capacity of 991 mAh g^(-1) after 500 cycles at the current density of 1.0 A g^(-1). The dis?charge capacity of the CYS?NiO/C microspheres after the 1000 th cycle at the current density of 2.0 A g^(-1) was 635 mAh g^(-1), and the capacity retention measured from the second cycle was 91%. The final discharge capacities of the CYS?NiO/C microspheres at the current densities of 0.5, 1.5, 3.0, 5.0, 7.0, and 10.0 A g^(-1) were 753, 648, 560, 490, 440, and 389 mAh g^(-1), respectively. The synergetic e ect of the coral?like yolk–shell structure with well?defined interconnected mesopores and highly conductive carbon resulted in the excellent Li+?ion storage properties of the CYS?NiO/C microspheres.
基金supported by the National Natural Science Foundation of China(Grant Nos.61222501 and 61335004)
文摘The electrical and optical properties of the indium tin oxide （ITO）/epoxy composite exhibit dramatic variations as functions of the ITO composition and ITO particle size. Sharp increases in the conductivity in the vicinity of a critical volume fraction have been found within the framework of percolation theory. A conductive and insulating transition model is extracted by the ITO particle network in the SEM image, and verified by the resistivity dependence on the temperature. The dependence of the optical transmittance on the particle size was studied. Further decreasing the ITO particle size could further improve the percolation threshold and light transparency of the composite film.
文摘Ceria-based heterostructure composite(CHC)has become a new stream to develop advanced low-temperature(300–600°C)solid oxide fuel cells(LTSOFCs)with excellent power outputs at 1000 mW cm−2 level.The state-ofthe-art ceria–carbonate or ceria–semiconductor heterostructure composites have made the CHC systems significantly contribute to both fundamental and applied science researches of LTSOFCs;however,a deep scientific understanding to achieve excellent fuel cell performance and high superionic conduction is still missing,which may hinder its wide application and commercialization.This review aims to establish a new fundamental strategy for superionic conduction of the CHC materials and relevant LTSOFCs.This involves energy band and built-in-field assisting superionic conduction,highlighting coupling effect among the ionic transfer,band structure and alignment impact.Furthermore,theories of ceria–carbonate,e.g.,space charge and multi-ion conduction,as well as new scientific understanding are discussed and presented for functional CHC materials.
基金the financial support from the Jiangsu Provincial Key Research and Development Program (Grant No. BE2019008)the Natural Science Foundation of China (Grant No. 51573103, 21274094 and 21304060)。
文摘Poly(decamethylene terephthalamide/decamethylene isophthalamide)-block-polyvinyl alcoho)(PA10 T/10 IPEG) copolymer/graphene oxide(GO) composites were prepared via in-situ melt polymerization and two different nano-filler addition approaches were compared. The relationship between the micro-structure and performance of the elastomer composites prepared by one-step and two-step methods was explored. The results show that the two-step method significantly promoted the dispersion of the GO in a polymer matrix, and facilitated the grafting of more hard molecular chains. Thus, the elastic modulus and tensile strength of the nanocomposite have been significantly improved by the presence of GO. This was because of the strong interaction between the functional groups on the surface of the GO and the hard molecular chains. This would be also be favorable to load transfer across the interface. Additionally, the elongation at the break of composites increased by 10% with the addition of a small amount of GO(0.2% wt). This is because hard domains tend to be enriched on the surface of GO in composites and act as a lubricating layer at the interface between the GO and matrix, leading to increased deformation ability. This work provides an effective strategy to prepare elastomer composites with high strength and toughness.
基金supported by the National Natural Science Foundation of China(Grants No.21067004 and No.21263005)the Technological Foundation of Jiangxi Province Education Office(No.GJJ12344)+1 种基金the Young Science and Technolgy Project of Jiangxi Province(No.20133BAB21003)the Young Scientist Training Project of Jiangxi Province(No.20122BCB23015)
文摘A series of novel Ni/CeOe-Al2O3 composite catalysts were synthesized by one-step citric acid complex method, The as-synthesized catalysts were characterized by N2 physical adsorption/desorption, X-ray diffraction （XRD）, Fourier transform infrared （FT-IR） spectroscopy, hydrogen temperature-programmed reduction （Hz-TPR）, X-ray photoelectron spectroscopy （XPS） and thermogravimetry analysis （TGA）. The effects of nickel content, calcination and reaction temperatures, gas hourly space velocity （GHSV） and inert gas dilution of N2 on their performance of catalytic partial oxidation of methane （CPOM） were investigated. Catalytic activity test results show that the highest methane conversion （〉85%）, the best selectivities to carbon monoxide （〉87%） and to hydrogen （〉95%）, the excellent stability and perfect Hz/CO ratio （2.0） can be obtained over Ni/CeO2-Al2O3 with 8 wt% Ni content calcined at 700 ℃ under the reaction condition of 750 ℃, CH4/O2 ratio of 2 ： 1 and gas hourly space velocity of 12000 mL.h-1 .g-1. Characterization results show that the good catalytic performance of this composite catalyst can be contributed to its large specific surface area （~108 m2.g-1）, small crystallite size, easy reducibility and low coking rate.
基金Ministry of Education and Science of the Russian Federation(14.613.21.0043)
文摘The experimental values of the enthalpy of formation of two isomeric 3,4-and 3,5-dinitro-1-(trinitromethyl)-1H-pyrazoles have been obtained(261.5±5.0and 246.4±6.7kJ/mol for crystalline 3,4-and 3,5-dinitro-1-(trinitromethyl)-1H-pyrazoles,respectively).The ballistic effectiveness of these potential oxidizers in composite solid propellants was studied.It is shown that these two oxidizers may be successfully applied in metal-free compositions or with a small content of metal.For the bottom stage 3,4-dinitro-1-(trinitromethyl)-1H-pyrazole is a bit better than 3,5-dinitro-1-(trinitromethyl)-1H-pyrazole,for the upper stage the both oxidizers show the equal ballistic parameters.These oxidizers allow to create metal-free solid composite propellants with the binder percentage not lower than 19%(volume fraction),with I3spequal to 256.5-257.0sat density equal to 1.72-1.74g/cm^3.
基金Project supported by the Doctoral Research Fund of Southwest University of Science and Technology(Grant No.20zx7104)the Sichuan Science and Technology Program(Grant No.2020ZYD055)the National Natural Science Foundation of China(Grant Nos.11905206 and 12075194)。
文摘Ti_(0.2)Zr_(0.2)Hf_(0.2)Nb_(0.2)Ta_(0.2)C-M_(t)C composite ceramic was prepared by hot press sintering,with the Ti_(0.2)Zr_(0.2)Hf_(0.2)Nb_(0.2)Ta_(0.2)C high-entropy carbide as the main phase.Secondary phase M_(x)C(M=Ti,Zr,Hf,Nb,Ta) was found to be distributed relatively uniform in the composite ceramic.The oxidation behavior of the ceramic was examined after exposure to 923 K and 1173 K.Morphology of the surface and cross sections of all oxidation samples were observed.The characteristics of the oxidation behavior of the high-entropy carbide and the secondary phase M_(x)C were compared and analyzed.The secondary phases(such as Ti-rich carbide or Hf-rich carbide) in the material were seriously oxidized at 923 K and 1173 K,which reflects the superior oxidation performance of the high-entropy carbide.The nano high-entropy oxides with Ti,Zr,Hf,Nb,Ta,and O elements were discovered by oxidation of the composite ceramic.This research will help deepen the understanding of the oxidation mechanism of high-entropy carbide and composite ceramic.
基金supported by grants from the National Natural Science Foundation of China(No. 21306106)the Open Foundation of the State Key Laboratory of Bioactive Seaweed Substances,Qingdao Brightmoon Seaweed Group Co., Ltd.(No. SKL-BASS1723)
文摘Bulk Ni-Mo composites were prepared by a simple solid reaction method and the hydrodeoxygenation activity of samples was examined. The test results showed that the Ni-Mo catalysts possessed high catalytic activity for hydrogenation of p-cresol under mild conditions. The XRD, N_2 isothermal adsorption, NH_3-TPD characterization analyses indicated that the excellent hydrogenation performance of Ni-Mo catalysts could be attributed to their incorporated Mo metal, the developed pore system, and the strong acidity.
文摘Titanium oxide films were prepared by annealing DC magnetron sputtered titanium films in an oxygen ambient. X-ray diffraction （XRD）, Auger electron spectroscopy （AES） sputter profiling, MCs^＋-mode secondary ion mass spectrometry （MCs^＋-SIMS） and atomic force microscopy （AFM） were employed, respectively, for the structural, com- positional and morphological characterization of the obtained films. For temperatures below 875 K, titanium films could not be fully oxidized within one hour. Above that temperature, the completely oxidized films were found to be rutile in structure. Detailed studies on the oxidation process at 925K were carried out for the understanding of the underlying mechanism of titanium dioxide （TiO2） formation by thermal oxidation. It was demonstrated that the formation of crystalline TiO2 could be divided into a short oxidation stage, followed by crystal forming stage. Relevance of this recognition was further discussed.
基金supported by National Natural Science Foundation of China (NO.0576023)Key Project of Science and Technology Department of Guangdong Province (NO.2008B010800036 NO.2008B010800037)
文摘Carbon nanotubes-Nafion （CNTs-Nation） composites were prepared by impregnated CNTs with Nation in ethanol solution and characterized by FT-IR. Pt-Ru catalysts supported on CNTs-Nafion composites were synthesized by microwave-assisted polyol process. The physical and electrochemical properties of the catalysts were characterized by X-ray diffraction （XRD）, transmission electron microscope （TEM）, CO stripping voltammetry, cyclic voltammetry （CV） and chronoamperometry （CA）. The results showed that the Nation incorporation in CNTs-Nation composites did not significantly alter the oxygen-containing groups on the CNTs surface. The Pt-Ru catalyst supported on CNTs-Nafion composites with 2 wt% Naton showed good dispersion and the best CO oxidation and methanol electro-oxidation activities.
基金supported by the National Natural Science Foundation of China (52002412 and 22072186)the Natural Science Foundation of Guangdong Province (2021A1515010575)the Fundamental Research Funds for the Central Universities, Sun Yat-sen University (23lgbj017)。
文摘Exploiting high-efficiency Ni-based materials for electrocatalytic urea oxidation reaction(UOR) is critical for urea-related technologies.The catalytic site density,intrinsic activity,charge transfer,and mass diffusion determine overall electrocatalytic efficiency.Simultaneous modulation over the above four factors promises advanced electrocatalysis,yet challenging.Herein we propose a systematic regulation tactic over composition and geometric structure,constructing a nanocomposite comprising Mn doped Ni_(3)N nanoparticles anchored on reduced graphene oxide(rGO/Mn-Ni_(3)N),achieving elegant integration of four design principles into one,thereby eminently boosting UOR.Particularly,Mn doping in Ni_(3)N can modulate electronic state to induce intrinsic activity regulation.Combining metallic Mn-Ni_(3)N with rGO to engineer hierarchical architecture not only promotes charge transfer,but also enriches active site population.Intriguingly,improved hydrophilicity could impart better electrolyte penetration and gas escape.Consequently,such system-optimized rGO/Mn-Ni_(3)N demonstrates state-of-the-art-level UOR electrocatalysis.This work offers a novel paradigm to create advanced catalysts via systematic and integrated modulation.
基金supported by the National Natural Science Foundation of China (No.21776156).
文摘High activity and productivity of MoVNbTeO_(x) catalyst are challenging tasks in oxidative dehydrogenation of ethane(ODHE)for industrial application.In this work,phase-pure M1 with 30 wt%CeO_(2) composite catalyst was treated by oxygen plasma to further enhance catalyst performance.The results show that the oxygen vacancies generated by the solid-state redox reaction between M1 and CeO_(2) capture active oxygen species in gas and transform V^(4+)to V^(5+)without damage to M1 structure.The space-time yield of ethylene of the plasma-treated catalyst was significantly increased,in which the catalyst shows an enhancement near~100% than that of phase-pure M1 at 400℃ for ODHE process.Plasma treatment for catalysts demonstrates an effective way to convert electrical energy into chemical energy in catalyst materials.Energy conversion is achieved by using the catalyst as a medium.
基金financial support from National Key Research&Development Project(2016YFE0126900)the National Natural Science Foundation of China(51672095)+2 种基金Hubei Province(2018AAA057)the EPSRC Capital for Great Technologies Grant EP/L017008/1the China Scholarship Council for funding(201806160178)。
文摘In this study,we successfully synthesized double perovskite-type oxide NdBa0.5Ca0.5Co1.5Fe0.5O5+δ(NBCCF)using a conventional wet chemical method as the oxygen electrode for reversible solid oxide electrochemical cells(RSOCs).The polarization resistance(Rp)of the composite electrode NBCCFGd0.1Ce0.9O2(GDC)is only 0.079Ωcm^2 at 800℃under air.The single cell based on NBCCF-GDC electrode displays a peak power density of 0.941 W/cm^2 in fuel cell mode and a low Rp value of 0.134Ωcm^2.In electrolysis cell mode,the cell displays an outstanding oxygen evolution reaction(OER)activity and shows current density as high as 0.92 A/cm^2 with 50 vol%AH(Absolute Humidity)at 800℃and applied voltage of 1.3 V.Most importantly,the cell exhibits admirable durability of 60 h both in electrolysis mode and fuel cell mode with distinguished reversibility.All these results suggest that NBCCF is a promising candidate electrode for RSOC.
基金financial support from the National Natural Science Foundation of China(grant no.21406052the Program for the Outstanding Young Talents of Hebei Province(grant no.BJ2014010)the Scientific Research Foundation for Selected Overseas Chinese Scholars,Ministry of Human Resources and Social Security of China(grant no.CG2015003002)
文摘The high-energy lithium/sulfur(Li/S) battery has become a very popular topic of research in recent years due to its high theoretical capacity of 1672 m Ah/g. However, the polysulfide shuttle effect remains of great concern with a great number of publications dedicated to its mitigation. In this contribution, a three-dimensional(3D) reduced graphene oxide/activated carbon(RGO/AC) film, synthesized by a simple hydrothermal method and convenient mechanical pressing, is sandwiched between the separator and the sulfur-based cathode, acting as a functional interlayer to capture and trap polysulfide species. Consequently, the Li/S cell with this interlayer shows an impressive initial discharge capacity of 1078 m Ah/g and a reversible capacity of 655 m Ah/g even after 100 cycles. The RGO/AC interlayer impedes the movement of polysulfide while providing unimpeded channels for lithium ion mass transfer. Therefore, the RGO/AC interlayer with a well-designed structure represents strong potential for high-performance Li/S batteries.
基金supported by the National Natural Science Foundation of China (51203071, 51363014 and 51362018)China Postdoctoral Science Foundation (2014M552509)+1 种基金the Key Project of Chinese Ministry of Education (212183)the Natural Science Funds for Distinguished Young Scholars of Gansu Province (1111RJDA012)
文摘This article reported the electrochemical behaviors of a novel hollow carbon microspheres/manganese dioxide nanosheets(micro-HC/nano-MnO2) composite prepared by an in situ self-limiting deposition method under hydrothermal condition. The results of scanning electron microscopy reveal that MnO2 nanosheets homogeneously grow onto the surface of micro-HC to form a loose-packed microstructure. The quantity of MnO2 required in the electrode layer has thereby been reduced significantly, and higher specific capacitances have been achieved. The micro-HC/nano-MnO2 electrode presents a high capacitance of 239.0 F g-1 at a current density of 5 m A cm-2, which is a strong promise for high-rate electrochemical capacitive energy storage applications.
文摘Natural intercalation of the graphite oxide, obtained as a product of Hummer＇s method, via ultra-sonication of water dispersed graphite oxide has been carried out to obtain graphene oxide（GO） and thermally reduced graphene oxide（RGO）.Here we report the effect of metallic nitrate on the oxidation properties of graphite and then formation of metallic oxide（MO） composites with GO and RGO for the first time. We observed a change in the efficiency of the oxidation process as we replaced the conventionally used sodium nitrate with that of nickel nitrate Ni（NO_3）_2, cadmium nitrate Cd（NO_3）_2,and zinc nitrate Zn（NO_3）_2. The structural properties were investigated by x-ray diffraction and observed the successful formation of composite of MO–GO and MO–RGO（M = Zn, Cd, Ni）. We sought to study the effect on the oxidation process through optical characterization via UV-Vis spectroscopy and Fourier Transform Infrared（FTIR） spectroscopy.Moreover, Thermo Gravimetric Analysis（TGA） was carried out to confirm 〉 90% weight loss in each process thus proving the reliability of the oxidation cycles. We have found that the nature of the oxidation process of graphite powder and its optical and electrochemical characteristics can be tuned by replacing the sodium nitrate（NaNO_3） by other metallic nitrates as Cd（NO_3）_2, Ni（NO_3）_2, and Zn（NO_3）_2. On the basis of obtained results, the synthesized GO and RGO may be expected as a promising material in antibacterial activity and in electrodes fabrication for energy devices such as solar cell, fuel cell,and super capacitors.
基金supported by the National Natural Science Foundation of China,NSFC(51772205,51772208)the General Program of Municipal Natural Science Foundation of Tianjin(17JCYBJC17000,17JCYBJC22700)。
文摘The emergency of high-power electrical appliances has put forward higher requirements for the power density of lithium-ion batteries.Vanadium oxides with large theoretical capacities and high operating voltages are considered as prospective alternatives for the cathode of a new generation of lithium-ion batteries.However,the poor rate and cycling performance caused by the sluggish electrons/lithium transportation,irreversible phase changes,vanadium dissolution and large volume changes during the repeated lithium intercalation/deintercalation hinder their commercial development.Several optimizing routes have been carried out and extensively explored to address these problems.Taking V_(2)O_(5),VO_(2)(B),V_(6)O_(13),and V_(2)O_(3)as examples,this article reviewed their crystal structures and lithium storage reactions.Besides,recent progress in modification methods for the electrochemical insufficiencies of vanadium oxides,including nanostructure,heterogeneous atom doping,composite and self-supported electrodes has been systematically summarized and finally,the challenges for the industrialization of vanadium oxide cathodes and their development opportunities are proposed.
