Based on the basis of analysis and interpretation of the products distribution of catalytic cracking of high acidic crude, the mechanism for decarboxylation of petroleum acids during FCC process was discussed. The pro...Based on the basis of analysis and interpretation of the products distribution of catalytic cracking of high acidic crude, the mechanism for decarboxylation of petroleum acids during FCC process was discussed. The protons originated from the Bronsted acid sites can combine with oxygen of the carbonyl groups with more negative charges to form reaction intermediates that can be subjected to cleavage at the weak bonds, leading to breaking of carboxylic groups from the carboxylic acids followed by its decomposition to form alkyl three-coordinated carbenium ions, CO and H2O. The Lewis acid as an electrophilic reagent can abstract carboxylic groups from carboxylic acids to subsequently release CO2.展开更多
Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NH...Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NHMC/Ni/NiO)nanocomposite for developing high-capacity LIBs anode materials through carbonization and selective etching strategies.The synthesized NMHC/Ni/NiO-0.33 composite exhibited a highly regular microstructure with well-dispersed Ni/NiO particles.The composite had a surface area of 408 m^(2)·g^(−1),a mesopore ratio of 75.0%,and a pyridine–nitrogen ratio of 58.9%.The introduction of nitrogen atoms reduced the disordered structure of lignin mesoporous carbon and enhanced its electrical conductivity,thus improving the lithium storage capabilities of the composite.Following 100 cycles at a current density of 0.2 A·g^(−1),the composite demonstrated enhanced Coulomb efficiency and rate performance,achieving a specific discharge capacity of 1230.9 mAh·g^(−1).At a high-current density of 1 A·g^(−1),the composite exhibited an excellent specific discharge capacity of 714.6 mAh·g^(−1).This study presents an innovative method for synthesizing high-performance anode materials of LIBs.展开更多
Considering the serious electromagnetic wave(EMW)pollution problems and complex application condition,there is a pressing need to amalgamate multiple functionalities within a single substance.However,the effective int...Considering the serious electromagnetic wave(EMW)pollution problems and complex application condition,there is a pressing need to amalgamate multiple functionalities within a single substance.However,the effective integration of diverse functions into designed EMW absorption materials still faces the huge challenges.Herein,reduced graphene oxide/carbon foams(RGO/CFs)with two-dimensional/three-dimensional(2D/3D)van der Waals(vdWs)heterostructures were meticulously engineered and synthesized utilizing an efficient methodology involving freeze-drying,immersing absorption,secondary freeze-drying,followed by carbonization treatment.Thanks to their excellent linkage effect of amplified dielectric loss and optimized impedance matching,the designed 2D/3D RGO/CFs vdWs heterostructures demonstrated commendable EMW absorption performances,achieving a broad absorption bandwidth of 6.2 GHz and a reflection loss of-50.58 dB with the low matching thicknesses.Furthermore,the obtained 2D/3D RGO/CFs vdWs heterostructures also displayed the significant radar stealth properties,good corrosion resistance performances as well as outstanding thermal insulation capabilities,displaying the great potential in complex and variable environments.Accordingly,this work not only demonstrated a straightforward method for fabricating 2D/3D vdWs heterostructures,but also outlined a powerful mixeddimensional assembly strategy for engineering multifunctional foams for electromagnetic protection,aerospace and other complex conditions.展开更多
To improve the catalytic performance of La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3)(LSCF)towards carbon soot,we utilized the impregnation method to incorporate Ag into the prepared LSCF catalyst.We conducted a series of cha...To improve the catalytic performance of La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3)(LSCF)towards carbon soot,we utilized the impregnation method to incorporate Ag into the prepared LSCF catalyst.We conducted a series of characterization tests and evaluated the soot catalytic activity of the composite catalyst by comparing it with the LaCoO_(3) group,LaFeO_(3) group,and catalyst-free group.The results indicate that the Ag-LSCF composite catalyst exhibits the highest soot catalytic activity,with the characteristic temperature values of 376.3,431.1,and 473.9℃at 10%,50%,and 90%carbon soot conversion,respectively.These values are 24.8,20.2,and 23.1℃lower than those of the LSCF group.This also shows that LSCF can improve the catalytic activity of soot after compounding with Ag,and reflects the necessity of using catalysts in soot combustion reaction.XPS characterization and BET test show that Ag-LSCF has more abundant surface-adsorbed oxygen species,larger specific surface area and pore volume than LSCF,which also proves that Ag-LSCF has higher soot catalytic activity.展开更多
Aerated drip irrigation(ADI)is an important practice for promoting soil fertility and crop productivity in greenhouse vegetable production,yet little research has comprehensively investigated its effects on the functi...Aerated drip irrigation(ADI)is an important practice for promoting soil fertility and crop productivity in greenhouse vegetable production,yet little research has comprehensively investigated its effects on the functional traits of carbon(C)-cycling microorganisms.In this study,we sought to assess the potential efficacy of ADI in increasing soil organic C(SOC)by changing soil microbial communities and the expressions of genes associated with C cycling.To this end,we adopted a metagenomic approach to compare the effects of ADI with three dissolved oxygen concentrations(10,15,and 20 mg L^(-1))during a three-season tomato cultivation experiment in northern China.The results revealed that the 10 mg L^(-1)treatment led to a significant increase in the abundance of korA/B genes(associated with the reductive tricarboxylic acid cycle)in the C fixation pathway,whereas the 15 mg L^(-1)treatment increased the abundances of cbbL/R and coxL/S genes associated with the Calvin cycle and carbon monoxide oxidation,respectively.In addition,based on a co-occurrence network analysis,we observed a positive correlation between cbbL and coxS.Interestingly,r-selected microorganisms,such as Proteobacteria and Actinobacteria,characterized by rapid cell multiplication and high biomass production,were identified as the primary contributors to C fixation and were the main predictors of SOC pools.In contrast,the 20 mg L^(-1)treatment was found to adversely influence C fixation,although the enhanced C degradation could be attributed to the extracellular enzymes secreted by K-selected microorganisms.Collectively,our findings indicate that ADI with dissolved oxygen concentrations 15 mg L^(-1)can promote SOC content by altering the life history strategies of r-selected microorganisms and genes associated with C fixation.These findings will provide valuable references for agroecosystem irrigation management,help improve soil fertility,and promote sustainable production.展开更多
The effect of a wide variety of metal oxide (MOx) supports has been discussed for CO oxidation on nanoparticulate gold catalysts. By using typical co‐precipitation and deposition–precipitation methods and under id...The effect of a wide variety of metal oxide (MOx) supports has been discussed for CO oxidation on nanoparticulate gold catalysts. By using typical co‐precipitation and deposition–precipitation methods and under identical calcination conditions, supported gold catalysts were prepared on a wide variety of MOx supports, and the temperature for 50%conversion was measured to qualita‐tively evaluate the catalytic activities of these simple MOx and supported Au catalysts. Furthermore, the difference in these temperatures for the simple MOx compared to the supported Au catalysts is plotted against the metal–oxygen binding energies of the support MOx. A clear volcano‐like correla‐tion between the temperature difference and the metal–oxygen binding energies is observed. This correlation suggests that the use of MOx with appropriate metal–oxygen binding energies (300–500 kJ/atom O) greatly improves the catalytic activity of MOx by the deposition of Au NPs.展开更多
Bimetallic oxides composites have received an increasing attention as promising adsorbents for aqueous phosphate (P) removal in recent years. In this study, a novel magnetic composite MZLCO was prepared by hybridizing...Bimetallic oxides composites have received an increasing attention as promising adsorbents for aqueous phosphate (P) removal in recent years. In this study, a novel magnetic composite MZLCO was prepared by hybridizing amorphous Zr-La (carbonate) oxides (ZLCO) with nano-FeOthrough a one-pot solvothermal method for efficient phosphate adsorption. Our optimum sample of MZLCO-45 exhibited a high Langmuir maximum adsorption capacity of 96.16 mg P/g and performed well even at low phosphate concentration. The phosphate adsorption kinetics by MZLCO-45 fitted well with the pseudo-second-order model, and the adsorption capacity could reach 79% of the ultimate value within the first 60 min. The phosphate adsorption process was highly p H-dependent, and MZLCO-45 performed well over a wide p H range of 2.0-8.0. Moreover, MZLCO-45 showed a strong selectivity to phosphate in the presence of competing ions (Cl^(-), NO_(3)^(-), SO_(4)^(2-), HCO_(3)^(-), Ca^(2+), and Mg^(2+)) and a good reusability using the eluent of Na OH/Na Cl mixture, then 64% adsorption capacity remained after ten recycles. The initial 2.0 mg P/L in municipal wastewater and surface water could be efficiently reduced to below 0.1mg P/L by 0.07 g/L MZLCO-45, and the phosphate removal efficiencies were 95.7% and 96.21%, respectively. Phosphate adsorption mechanisms by MZLCO-45 could be attributed to electrostatic attraction and the inner-sphere complexation via ligand exchange forming Zr/La-O-P, -OH and CO_(3)^(2-)groups on MZLCO-45 surface played important roles in the ligand exchange process. The existence of oxygen vacancies could accelerate the phosphate absorption rate of the MZLCO-45 composites.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
In-situ growing carbon nanotubes (CNTs) directly on carbon fibers (CFs) always lead to a degraded tensile strength of CFs and then a poor fiber-dominated mechanical property of carbon/carbon composites (C/ Cs). ...In-situ growing carbon nanotubes (CNTs) directly on carbon fibers (CFs) always lead to a degraded tensile strength of CFs and then a poor fiber-dominated mechanical property of carbon/carbon composites (C/ Cs). To solve this issue, here, a novel carbon fiber-based multiscale reinforcement is reported. To synthesize it, carbon fibers (CFs) have been first grafted by graphene oxide (GO), and then carbon nanotubes (CNTs) have been in-situ grown on GO-grafted CFs by catalytic chemical vapor deposition. Characterizations on this novel reinforcement show that GO grafting cannot only nondestructively improve the surface chemical activity of CFs but also protect CFs against the high-temperature corrosion of metal catalyst during CNT growth, which maintains their tensile properties. Tensile property tests for unidirectional C/Cs with different preforms show that this novel reinforcement can endow C/C with improved tensile properties, 32% and 87% higher than that of pure C/C and C/C only doped with in-situ grown CNTs. This work would open up a possibility to fabricate multiscale C/Cs with excellent global performance.展开更多
A series of Fe2O3/Al2O3, Fe2O3/CeO2, Ce0.7Zr0.3O2, and Fe2O3/Ce1-xZrxO2(x = 0.1–0.4) oxides was prepared and their physicochemical features were investigated by X-ray diffraction(XRD), transmission electron micro...A series of Fe2O3/Al2O3, Fe2O3/CeO2, Ce0.7Zr0.3O2, and Fe2O3/Ce1-xZrxO2(x = 0.1–0.4) oxides was prepared and their physicochemical features were investigated by X-ray diffraction(XRD), transmission electron microscope(TEM), and H2-temperature-programmed reduction(H2-TPR) techniques. The gas–solid reactions between these oxides and methane for syngas generation as well as the catalytic performance for selective oxidation of carbon deposition in O2-enriched atmosphere were investigated in detail. The results show that the samples with the presence of Fe2O3show much higher activity for methane oxidation compared with the Ce0.7Zr0.3O2solid solution,while the CeO2-contained samples represent higher CO selectively in methane oxidation than the Fe2O3/Al2O3sample. This suggests that the iron species should be the active sites for methane activation, and the cerium oxides provide the oxygen source for the selective oxidation of the activated methane to syngas during the reaction between methane and Fe2O3/Ce0.7Zr0.3O2. For the oxidation process of the carbon deposition, the CeO2-containing samples show much higher CO selectivity than the Fe2O3/Al2O3sample, which indicates that the cerium species should play a very important role in catalyzing the carbon selective oxidation to CO. The presence of the Ce–Zr–O solid solution could induce the growth direction of the carbonfilament, resulting in a loose contact between the carbon filament and the catalyst. This results in abundant exposed active sites for catalyzing carbon oxidation, strongly improving the oxidation rate of the carbon deposition over this sample. In addition, the Fe2O3/Ce0.7Zr0.3O2also represents much higher selectivity(ca. 97 %) for the conversion of carbon to CO than the Fe2O3/CeO2sample, which can be attributed to the higher concentration of reduced cerium sites on this sample. The increase of the Zr content in the Fe2O3/Ce1-xZrxO2samples could improve the reactivity of the materials for methane oxidation, but it also reduces the selectivity for CO formation.展开更多
Direct carbon solid oxide fuel cells(DC-SOFCs)are promising,green,and efficient power-generating devices that are fueled by solid carbons and comprise all-solid-state structures.Developing suitable anode materials for...Direct carbon solid oxide fuel cells(DC-SOFCs)are promising,green,and efficient power-generating devices that are fueled by solid carbons and comprise all-solid-state structures.Developing suitable anode materials for DC-SOFCs is a substantial scientific challenge.Herein we investigated the use of La_(0.75)Sr_(0.25)Cr_(0.5)Mn_(0.5)O_(3)-δ−Ce_(0.8)Gd_(0.2)O_(1.9)(LSCM−GDC)composite electrodes as anodes for La_(0.9)Sr_(0.1)Ga_(0.8)Mg_(0.2)O_(3)-δelectrolyte-based DC-SOFCs,with Camellia oleifera shell char as the carbon fuel.The LSCM−GDC-anode DC-SOFC delivered a maximum power density of 221 mW/cm^(2) at 800℃ and it significantly improved to 425 mW/cm^(2) after Ni nanoparticles were introduced into the LSCM−GDC anode through wet impregnation.The microstructures of the prepared anodes were characterized,and the stability of the anode in a DC-SOFC and the influence of catalytic activity on open circuit voltage were studied.The above results indicate that LSCM–GDC anode is promising to be applied in DC-SOFCs.展开更多
The oxidation kinetics and composition of oxide scales on low carbon steel (SPHC) were studied during i- sothermal oxidation. Thermogravimetric analyzer (TGA) was used to simulate isothermal oxidation process of S...The oxidation kinetics and composition of oxide scales on low carbon steel (SPHC) were studied during i- sothermal oxidation. Thermogravimetric analyzer (TGA) was used to simulate isothermal oxidation process of SPHC for 240 min under air condition, and the temperature range was from 500 to 900 ℃. Scanning electron microscope (SEM) was used to observe cross-sectional scale morphology and analyze composition distribution of oxide scales. The morphology of oxide scale was classical three-layer structure. Fe2 03 developed as whiskers at the outermost lay- er, and interlayer was perforated-plate Fe3 04 while innermost layer was pyramidal FeO. From the oxidation curves, the oxidation mass gain per unit area with time was of parabolic relation and oxidation rate slowed down. On the ba- sis of experimental data, the isothermal oxidation kinetics model was derived and oxidation activation energy of SPHC steel was 127. 416 kJ/mol calculated from kinetics data.展开更多
The invasions of the alien species such as Spartina alterniflora along the northern Jiangsu coastlines have posed a threat to biodiversity and the ecosystem function.Yet,limited attention has been given to their poten...The invasions of the alien species such as Spartina alterniflora along the northern Jiangsu coastlines have posed a threat to biodiversity and the ecosystem function.Yet,limited attention has been given to their potential influence on greenhouse gas(GHG) emissions,including the diurnal variations of GHG fluxes that are fundamental in estimating the carbon and nitrogen budget.In this study,we examined the diurnal variation in fluxes of carbon dioxide(CO_2),methane(CH_4),and nitrous oxide(N2O) from a S.alterniflora intertidal flat in June,October,and December of 2013 and April of 2014 representing the summer,autumn,winter,and spring seasons,respectively.We found that the average CH_4 fluxes on the diurnal scale were positive during the growing season while negative otherwise.The tidal flat of S.alterniflora acted as a source of CH_4 in summer(June) and a combination of source and sink in other seasons.We observed higher diurnal variations in the CO_2 and N_2O fluxes during the growing season(1 536.5 mg CO_2 m^(–2) h^(–1) and 25.6 μg N_2O m^(–2) h^(–1)) compared with those measured in the non-growing season(379.1 mg CO_2 m^(–2) h^(–1) and 16.5 μg N_2O m^(–2) h^(–1)).The mean fluxes of CH_4 were higher at night than that in the daytime during all the seasons but October.The diurnal variation in the fluxes of CO_2 in June and N_2O in December fluctuated more than that in October and April.However,two peak curves in October and April were observed for the diurnal changes in CO_2 and N_2O fluxes(prominent peaks were found in the morning of October and in the afternoon of April,respectively).The highest diurnal variation in the N_2O fluxes took place at 15:00(86.4 μg N_2O m^(–2) h^(–1)) in June with an unimodal distribution.Water logging in October increased the emission of CO_2(especially at nighttime),yet decreased N_2O and CH_4 emissions to a different degree on the daily scale because of the restrained diffusion rates of the gases.The seasonal and diurnal variations of CH_4 and CO_2 fluxes did not correlate to the air and soil temperatures,whereas the seasonal and diurnal variation of the fluxes of N_2O in June exhibited a significant correlation with air temperature.When N_2O and CH_4 fluxes were converted to CO_2-e equivalents,the emissions of N_2O had a remarkable potential to impact the global warming.The mean daily flux(MF) and total daily flux(TDF) were higher in the growing season,nevertheless,the MF and TDF of CO_2 were higher in October and those of CH_4 and N_2O were higher in June.In spite of the difference in the optimal sampling times throughout the observation period,our results obtained have implications for sampling and scaling strategies in estimating the GHG fluxes in coastal saline wetlands.展开更多
Poly(amide-6-b-ethylene oxide)(Pebax1657)/1-butyl-3-methylimidazo-lium bis[trifluoromethyl)sulfonyl]-imide([Bmim][Tf2N]) blend membranes with different [Bmim][Tf2N] contents were prepared via solution casting a...Poly(amide-6-b-ethylene oxide)(Pebax1657)/1-butyl-3-methylimidazo-lium bis[trifluoromethyl)sulfonyl]-imide([Bmim][Tf2N]) blend membranes with different [Bmim][Tf2N] contents were prepared via solution casting and solvent evaporation method. The permeation properties of the blend membranes for CO2, N2,CH4 and H2 were studied, and the physical properties were characterized by differential scanning calorimeter(DSC) and X-ray diffraction(XRD). Results showed that [Bmim][Tf2N] was dispersed as amorphous phase in the blend membranes, which caused the decrease of Tg(PE) and crystallinity(PA). With the addition of [Bmim][Tf2N], the CO2 permeability increased and reached up to approximately 286 Barrer at 40 wt%[Bmim][Tf2N], which was nearly double that of pristine Pebax1657 membrane. The increase of CO2 permeability may be attributed to high intrinsic permeability of [Bmim][Tf2N], the increase of fractional free of volume(FFV) and plasticization effect. However, the CO2 permeability reduced firstly when the [Bmim][Tf2N]content was below 10 wt%, which may be due to that the small ions of [Bmim][Tf2N] in the gap of polymer chain inhibited the flexibility of polymer chain; the interaction between Pebax1657 and [Bmim][Tf2N]decreased the content of EO units available for CO2 transport and led to a more compact structure. For Pebax1657/[Bmim][Tf2N] blend membranes, the permeabilities of N2, H2 and CH4decreased with the increase of feed pressure due to the hydrostatic pressure effect, while CO2 permeability increased with the increase of feed pressure for that the CO2-induced plasticization effect was stronger than hydrostatic pressure effect.展开更多
Graphene oxide (GO)-multiwalled carbon nanotube (MWCNT) composite was synthesized and characterized by X-ray diffraction, atomic force microscopy, scanning electron microscopy, micro Raman, Fourier transform infra...Graphene oxide (GO)-multiwalled carbon nanotube (MWCNT) composite was synthesized and characterized by X-ray diffraction, atomic force microscopy, scanning electron microscopy, micro Raman, Fourier transform infrared and ultraviolet-visible near infrared spectroscopy techniques. Spectral characteris- tics of cladding modified fiber optic gas sensors were studied for various concentrations of ammonia, ethanol and methanol at 27 ℃. Thickness of the gas sensing layer was controlled by varying the concentration of composite in ethanol medium (0.5 and 1 mg/mL) for three times dipping process. The O.S mg/ mL concentrated GO-MWCNT coated sensor showed 1.20, 1.40 and 1.15 times higher sensitivity than the GO coated sensor for ammonia, ethanol and methanol vapors, respectively. Furthermore, it exhibited 1.50, 1.80 and 1.80 times better sensitivity than 1 mg/mL concentrated GO-MWCNT coated sensor for ammonia, ethanol and methanol vapors, respectively. The presence of functional groups in GO increased the sen- sitivity. This is mainly attributed to the effective electron charge transfer between the composite materials and analytes.展开更多
The collection of different cations in the A and B sites of ABO3 was explored for the regularity of perovskites phase formability.Here,Sr2?,La3?,and Ce4?are selected as the cations of site A.The site B is considere...The collection of different cations in the A and B sites of ABO3 was explored for the regularity of perovskites phase formability.Here,Sr2?,La3?,and Ce4?are selected as the cations of site A.The site B is considered to be Mn or Co cations.XRD analysis and Fourier transform infrared spectroscopy results confirm the formation of perovskite structure for catalysts in which La3?and Sr2?are considered as the cations of site A.Ceria is detected as the main crystalline phase when Ce4?is selected to be cation of site A.It is found that the octahedral factor(rB/rO) takes the same important role as the tolerance factor to form cubic perovskite.Average crystallite size of the products was calculated by data of the XRD and measured by the TEM analysis.Results of the XRD and TEM studies were supported by the study of the particles size distribution,which was carried out in a particle size analyzer.The perovskite samples were also used for stoichiometric oxidation of carbon monoxide with air.展开更多
To develop efficient catalysts for ambient carbon monoxide(CO)oxidation is significant for indoor air purification and also for many industrial applications.In this work,the catalytic activity for CO oxidation were en...To develop efficient catalysts for ambient carbon monoxide(CO)oxidation is significant for indoor air purification and also for many industrial applications.In this work,the catalytic activity for CO oxidation were enhanced by tuning the metal-support interaction of Ru/CeO_(2)catalysts.A series of Ru/CeO_(2)catalysts were synthesized by an impregnation method with calcination at 100,200,400 and 600℃,respectively,to regulate the Ru-CeO_(2)interaction.We discovered that low temperature calcination(100℃)induced more Ru-O-Ce bonds and stronger Ru-CeO_(2)interaction,while high temperature calcination(≥400℃)caused the agglomeration of Ru species with more Ru-O-Ru bonds and weaker Ru-CeO_(2)interaction,resulting in the lower redox capacity of these catalysts,as well as lower catalytic activity for CO oxidation.Only calcination at moderate 200℃ can induce the moderate interaction between Ru species and CeO_(2)support,which can keep the high dispersion of RuO_(x)species with the high redox capacity,thus leading to complete elimination of 500 ppm CO at room temperature on Ru/Ce-200 catalyst.展开更多
Pd/C catalysts were prepared by deposited Pd nanoparticles (NPs) on different carbon supports including activated carbon (AC), graphite oxide (GO), and reduced graphite oxide (rGO) using sol-immobilization met...Pd/C catalysts were prepared by deposited Pd nanoparticles (NPs) on different carbon supports including activated carbon (AC), graphite oxide (GO), and reduced graphite oxide (rGO) using sol-immobilization method. Through transmission electron microscopy, powder X-ray di raction, and X-ray photoelectron spectroscopy, the role of the carbon supports for the catalytic performances of Pd/C catalysts was examined in selective hydrogenation of acetylene. The results indicate that Pd/AC exhibited higher activity and selectivity than Pd/GO and Pd/rGO in the gas phase selective hydrogenation of acetylene. Thermal and chemical treatment of AC supports also have some effect on the catalytic performance of Pd/AC catalysts. The differences in the activity and selectivity of various Pd/C catalysts were partly attributed to the metal-support interaction.展开更多
Nanostructured gold catalyst supported on metal oxide is highly active for the CO oxidation reac‐tion. In this work, a new type of oxide support, zinc tin oxide, has been used to deposit 0.7 wt%Au via a deposition‐p...Nanostructured gold catalyst supported on metal oxide is highly active for the CO oxidation reac‐tion. In this work, a new type of oxide support, zinc tin oxide, has been used to deposit 0.7 wt%Au via a deposition‐precipitation method. The textural properties of Zn2SnO4 support have been tuned by varying the molar ratio between base (N2H4·H2O) and metal ion (Zn2+) to be 4/1, 8/1 and 16/1. The catalytic tests for CO oxidation reaction revealed that the reactivity on Au‐Zn2SnO4 with N2H4·H2O/Zn2+ = 8/1 was the highest, while the reactivity on Au‐Zn2SnO4 with N2H4·H2O/Zn2+ =16/1 was almost identical to that of the pure support. Both fresh and used catalysts have been characterized by multiple techniques including nitrogen adsorption‐desorption, X‐ray diffraction, transmission electron microscopy, high‐angle annular dark‐field scanning transmission electron microscopy, X‐ray photoelectron spectroscopy, X‐ray adsorption fine structure, and tempera‐ture‐programmed reduction by hydrogen. These demonstrated that the textural properties, espe‐cially pore volume and pore size distribution, of Zn2SnO4 play crucial roles in the averaged size of gold nanoparticles, and thus determine the catalytic activity of Au‐Zn2SnO4 for CO oxidation.展开更多
文摘Based on the basis of analysis and interpretation of the products distribution of catalytic cracking of high acidic crude, the mechanism for decarboxylation of petroleum acids during FCC process was discussed. The protons originated from the Bronsted acid sites can combine with oxygen of the carbonyl groups with more negative charges to form reaction intermediates that can be subjected to cleavage at the weak bonds, leading to breaking of carboxylic groups from the carboxylic acids followed by its decomposition to form alkyl three-coordinated carbenium ions, CO and H2O. The Lewis acid as an electrophilic reagent can abstract carboxylic groups from carboxylic acids to subsequently release CO2.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.22278092,22078116 and 22222805)Guangdong Provincial Key Research and Development Program(No.2020B1111380002)+2 种基金Science and Technology Research Project of Guangzhou(Nos.2023A03J0034,2023A04J0077 and 202102020467)State Key Laboratory of Pulp and Paper Engineering(No.202313)Key Discipline of Materials Science and Engineering,Bureau of Education of Guangzhou(No.202255464).
文摘Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NHMC/Ni/NiO)nanocomposite for developing high-capacity LIBs anode materials through carbonization and selective etching strategies.The synthesized NMHC/Ni/NiO-0.33 composite exhibited a highly regular microstructure with well-dispersed Ni/NiO particles.The composite had a surface area of 408 m^(2)·g^(−1),a mesopore ratio of 75.0%,and a pyridine–nitrogen ratio of 58.9%.The introduction of nitrogen atoms reduced the disordered structure of lignin mesoporous carbon and enhanced its electrical conductivity,thus improving the lithium storage capabilities of the composite.Following 100 cycles at a current density of 0.2 A·g^(−1),the composite demonstrated enhanced Coulomb efficiency and rate performance,achieving a specific discharge capacity of 1230.9 mAh·g^(−1).At a high-current density of 1 A·g^(−1),the composite exhibited an excellent specific discharge capacity of 714.6 mAh·g^(−1).This study presents an innovative method for synthesizing high-performance anode materials of LIBs.
基金provided by Guizhou Provincial Science and Technology Projects for Platform and Talent Team Plan(GCC[2023]007)Fok Ying Tung Education Foundation(171095)National Natural Science Foundation of China(11964006).
文摘Considering the serious electromagnetic wave(EMW)pollution problems and complex application condition,there is a pressing need to amalgamate multiple functionalities within a single substance.However,the effective integration of diverse functions into designed EMW absorption materials still faces the huge challenges.Herein,reduced graphene oxide/carbon foams(RGO/CFs)with two-dimensional/three-dimensional(2D/3D)van der Waals(vdWs)heterostructures were meticulously engineered and synthesized utilizing an efficient methodology involving freeze-drying,immersing absorption,secondary freeze-drying,followed by carbonization treatment.Thanks to their excellent linkage effect of amplified dielectric loss and optimized impedance matching,the designed 2D/3D RGO/CFs vdWs heterostructures demonstrated commendable EMW absorption performances,achieving a broad absorption bandwidth of 6.2 GHz and a reflection loss of-50.58 dB with the low matching thicknesses.Furthermore,the obtained 2D/3D RGO/CFs vdWs heterostructures also displayed the significant radar stealth properties,good corrosion resistance performances as well as outstanding thermal insulation capabilities,displaying the great potential in complex and variable environments.Accordingly,this work not only demonstrated a straightforward method for fabricating 2D/3D vdWs heterostructures,but also outlined a powerful mixeddimensional assembly strategy for engineering multifunctional foams for electromagnetic protection,aerospace and other complex conditions.
文摘To improve the catalytic performance of La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3)(LSCF)towards carbon soot,we utilized the impregnation method to incorporate Ag into the prepared LSCF catalyst.We conducted a series of characterization tests and evaluated the soot catalytic activity of the composite catalyst by comparing it with the LaCoO_(3) group,LaFeO_(3) group,and catalyst-free group.The results indicate that the Ag-LSCF composite catalyst exhibits the highest soot catalytic activity,with the characteristic temperature values of 376.3,431.1,and 473.9℃at 10%,50%,and 90%carbon soot conversion,respectively.These values are 24.8,20.2,and 23.1℃lower than those of the LSCF group.This also shows that LSCF can improve the catalytic activity of soot after compounding with Ag,and reflects the necessity of using catalysts in soot combustion reaction.XPS characterization and BET test show that Ag-LSCF has more abundant surface-adsorbed oxygen species,larger specific surface area and pore volume than LSCF,which also proves that Ag-LSCF has higher soot catalytic activity.
基金financially supported by the National Natural Science Foundation of China(Nos.52379048 and 52079112)the Key Research and Development Program of Shaanxi Province,China(No.2022ZDLNY03-03)the Major Science and Technology Engineering Innovation Project of Shandong Province,China(No.2020CXGC 010808)。
文摘Aerated drip irrigation(ADI)is an important practice for promoting soil fertility and crop productivity in greenhouse vegetable production,yet little research has comprehensively investigated its effects on the functional traits of carbon(C)-cycling microorganisms.In this study,we sought to assess the potential efficacy of ADI in increasing soil organic C(SOC)by changing soil microbial communities and the expressions of genes associated with C cycling.To this end,we adopted a metagenomic approach to compare the effects of ADI with three dissolved oxygen concentrations(10,15,and 20 mg L^(-1))during a three-season tomato cultivation experiment in northern China.The results revealed that the 10 mg L^(-1)treatment led to a significant increase in the abundance of korA/B genes(associated with the reductive tricarboxylic acid cycle)in the C fixation pathway,whereas the 15 mg L^(-1)treatment increased the abundances of cbbL/R and coxL/S genes associated with the Calvin cycle and carbon monoxide oxidation,respectively.In addition,based on a co-occurrence network analysis,we observed a positive correlation between cbbL and coxS.Interestingly,r-selected microorganisms,such as Proteobacteria and Actinobacteria,characterized by rapid cell multiplication and high biomass production,were identified as the primary contributors to C fixation and were the main predictors of SOC pools.In contrast,the 20 mg L^(-1)treatment was found to adversely influence C fixation,although the enhanced C degradation could be attributed to the extracellular enzymes secreted by K-selected microorganisms.Collectively,our findings indicate that ADI with dissolved oxygen concentrations 15 mg L^(-1)can promote SOC content by altering the life history strategies of r-selected microorganisms and genes associated with C fixation.These findings will provide valuable references for agroecosystem irrigation management,help improve soil fertility,and promote sustainable production.
文摘The effect of a wide variety of metal oxide (MOx) supports has been discussed for CO oxidation on nanoparticulate gold catalysts. By using typical co‐precipitation and deposition–precipitation methods and under identical calcination conditions, supported gold catalysts were prepared on a wide variety of MOx supports, and the temperature for 50%conversion was measured to qualita‐tively evaluate the catalytic activities of these simple MOx and supported Au catalysts. Furthermore, the difference in these temperatures for the simple MOx compared to the supported Au catalysts is plotted against the metal–oxygen binding energies of the support MOx. A clear volcano‐like correla‐tion between the temperature difference and the metal–oxygen binding energies is observed. This correlation suggests that the use of MOx with appropriate metal–oxygen binding energies (300–500 kJ/atom O) greatly improves the catalytic activity of MOx by the deposition of Au NPs.
基金supported by the Beijing Municipal Science and Technology Project (No. Z181100005518007)the National Key Research and Development Program of China (No. 2017YFC0505303)+1 种基金the National Natural Science Foundation of China (Nos. 51978054 and 51678053)Beijing Municipal Education Commission through the Innovative Transdisciplinary Program ‘Ecological Restoration Engineering’ (No. GJJXK210102)。
文摘Bimetallic oxides composites have received an increasing attention as promising adsorbents for aqueous phosphate (P) removal in recent years. In this study, a novel magnetic composite MZLCO was prepared by hybridizing amorphous Zr-La (carbonate) oxides (ZLCO) with nano-FeOthrough a one-pot solvothermal method for efficient phosphate adsorption. Our optimum sample of MZLCO-45 exhibited a high Langmuir maximum adsorption capacity of 96.16 mg P/g and performed well even at low phosphate concentration. The phosphate adsorption kinetics by MZLCO-45 fitted well with the pseudo-second-order model, and the adsorption capacity could reach 79% of the ultimate value within the first 60 min. The phosphate adsorption process was highly p H-dependent, and MZLCO-45 performed well over a wide p H range of 2.0-8.0. Moreover, MZLCO-45 showed a strong selectivity to phosphate in the presence of competing ions (Cl^(-), NO_(3)^(-), SO_(4)^(2-), HCO_(3)^(-), Ca^(2+), and Mg^(2+)) and a good reusability using the eluent of Na OH/Na Cl mixture, then 64% adsorption capacity remained after ten recycles. The initial 2.0 mg P/L in municipal wastewater and surface water could be efficiently reduced to below 0.1mg P/L by 0.07 g/L MZLCO-45, and the phosphate removal efficiencies were 95.7% and 96.21%, respectively. Phosphate adsorption mechanisms by MZLCO-45 could be attributed to electrostatic attraction and the inner-sphere complexation via ligand exchange forming Zr/La-O-P, -OH and CO_(3)^(2-)groups on MZLCO-45 surface played important roles in the ligand exchange process. The existence of oxygen vacancies could accelerate the phosphate absorption rate of the MZLCO-45 composites.
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 (Nos.51432008,51502242,U1435202,and 51202194)the Research Fund for the Doctoral Program of Higher Education of China (No.20126102110013)the Key Grant Project of Chinese Ministry of Education (No.313047)
文摘In-situ growing carbon nanotubes (CNTs) directly on carbon fibers (CFs) always lead to a degraded tensile strength of CFs and then a poor fiber-dominated mechanical property of carbon/carbon composites (C/ Cs). To solve this issue, here, a novel carbon fiber-based multiscale reinforcement is reported. To synthesize it, carbon fibers (CFs) have been first grafted by graphene oxide (GO), and then carbon nanotubes (CNTs) have been in-situ grown on GO-grafted CFs by catalytic chemical vapor deposition. Characterizations on this novel reinforcement show that GO grafting cannot only nondestructively improve the surface chemical activity of CFs but also protect CFs against the high-temperature corrosion of metal catalyst during CNT growth, which maintains their tensile properties. Tensile property tests for unidirectional C/Cs with different preforms show that this novel reinforcement can endow C/C with improved tensile properties, 32% and 87% higher than that of pure C/C and C/C only doped with in-situ grown CNTs. This work would open up a possibility to fabricate multiscale C/Cs with excellent global performance.
基金financially supported by the National Natural Science Foundation of China (Nos. 51004060, 51104074, and 51174105)the Natural Science Foundation of Yunnan Province (No. 2010ZC018)
文摘A series of Fe2O3/Al2O3, Fe2O3/CeO2, Ce0.7Zr0.3O2, and Fe2O3/Ce1-xZrxO2(x = 0.1–0.4) oxides was prepared and their physicochemical features were investigated by X-ray diffraction(XRD), transmission electron microscope(TEM), and H2-temperature-programmed reduction(H2-TPR) techniques. The gas–solid reactions between these oxides and methane for syngas generation as well as the catalytic performance for selective oxidation of carbon deposition in O2-enriched atmosphere were investigated in detail. The results show that the samples with the presence of Fe2O3show much higher activity for methane oxidation compared with the Ce0.7Zr0.3O2solid solution,while the CeO2-contained samples represent higher CO selectively in methane oxidation than the Fe2O3/Al2O3sample. This suggests that the iron species should be the active sites for methane activation, and the cerium oxides provide the oxygen source for the selective oxidation of the activated methane to syngas during the reaction between methane and Fe2O3/Ce0.7Zr0.3O2. For the oxidation process of the carbon deposition, the CeO2-containing samples show much higher CO selectivity than the Fe2O3/Al2O3sample, which indicates that the cerium species should play a very important role in catalyzing the carbon selective oxidation to CO. The presence of the Ce–Zr–O solid solution could induce the growth direction of the carbonfilament, resulting in a loose contact between the carbon filament and the catalyst. This results in abundant exposed active sites for catalyzing carbon oxidation, strongly improving the oxidation rate of the carbon deposition over this sample. In addition, the Fe2O3/Ce0.7Zr0.3O2also represents much higher selectivity(ca. 97 %) for the conversion of carbon to CO than the Fe2O3/CeO2sample, which can be attributed to the higher concentration of reduced cerium sites on this sample. The increase of the Zr content in the Fe2O3/Ce1-xZrxO2samples could improve the reactivity of the materials for methane oxidation, but it also reduces the selectivity for CO formation.
基金Project(2019YFC1907405)supported by the National Key R&D Program of ChinaProject(GJJ200809)supported by the Education Department Project Fund of Jiangxi Province,ChinaProject(2020BAB214021)supported by the Natural Science Foundation of Jiangxi Province,China。
文摘Direct carbon solid oxide fuel cells(DC-SOFCs)are promising,green,and efficient power-generating devices that are fueled by solid carbons and comprise all-solid-state structures.Developing suitable anode materials for DC-SOFCs is a substantial scientific challenge.Herein we investigated the use of La_(0.75)Sr_(0.25)Cr_(0.5)Mn_(0.5)O_(3)-δ−Ce_(0.8)Gd_(0.2)O_(1.9)(LSCM−GDC)composite electrodes as anodes for La_(0.9)Sr_(0.1)Ga_(0.8)Mg_(0.2)O_(3)-δelectrolyte-based DC-SOFCs,with Camellia oleifera shell char as the carbon fuel.The LSCM−GDC-anode DC-SOFC delivered a maximum power density of 221 mW/cm^(2) at 800℃ and it significantly improved to 425 mW/cm^(2) after Ni nanoparticles were introduced into the LSCM−GDC anode through wet impregnation.The microstructures of the prepared anodes were characterized,and the stability of the anode in a DC-SOFC and the influence of catalytic activity on open circuit voltage were studied.The above results indicate that LSCM–GDC anode is promising to be applied in DC-SOFCs.
基金Sponsored by National Natural Science Foundation of China(51204047)National Key Technology Research and Development Program in 12th Five-year Plan of China(2011BAE13B04)The Fundamental Research Funds for the Central Universities of China(N100307006)
文摘The oxidation kinetics and composition of oxide scales on low carbon steel (SPHC) were studied during i- sothermal oxidation. Thermogravimetric analyzer (TGA) was used to simulate isothermal oxidation process of SPHC for 240 min under air condition, and the temperature range was from 500 to 900 ℃. Scanning electron microscope (SEM) was used to observe cross-sectional scale morphology and analyze composition distribution of oxide scales. The morphology of oxide scale was classical three-layer structure. Fe2 03 developed as whiskers at the outermost lay- er, and interlayer was perforated-plate Fe3 04 while innermost layer was pyramidal FeO. From the oxidation curves, the oxidation mass gain per unit area with time was of parabolic relation and oxidation rate slowed down. On the ba- sis of experimental data, the isothermal oxidation kinetics model was derived and oxidation activation energy of SPHC steel was 127. 416 kJ/mol calculated from kinetics data.
基金The National Basic Research Program of China under contract No.2013CB956503the State Oceanic Administration People’s Republic of China under contract No.201005006the National Natural Science Foundation of China under contract No.41471413
文摘The invasions of the alien species such as Spartina alterniflora along the northern Jiangsu coastlines have posed a threat to biodiversity and the ecosystem function.Yet,limited attention has been given to their potential influence on greenhouse gas(GHG) emissions,including the diurnal variations of GHG fluxes that are fundamental in estimating the carbon and nitrogen budget.In this study,we examined the diurnal variation in fluxes of carbon dioxide(CO_2),methane(CH_4),and nitrous oxide(N2O) from a S.alterniflora intertidal flat in June,October,and December of 2013 and April of 2014 representing the summer,autumn,winter,and spring seasons,respectively.We found that the average CH_4 fluxes on the diurnal scale were positive during the growing season while negative otherwise.The tidal flat of S.alterniflora acted as a source of CH_4 in summer(June) and a combination of source and sink in other seasons.We observed higher diurnal variations in the CO_2 and N_2O fluxes during the growing season(1 536.5 mg CO_2 m^(–2) h^(–1) and 25.6 μg N_2O m^(–2) h^(–1)) compared with those measured in the non-growing season(379.1 mg CO_2 m^(–2) h^(–1) and 16.5 μg N_2O m^(–2) h^(–1)).The mean fluxes of CH_4 were higher at night than that in the daytime during all the seasons but October.The diurnal variation in the fluxes of CO_2 in June and N_2O in December fluctuated more than that in October and April.However,two peak curves in October and April were observed for the diurnal changes in CO_2 and N_2O fluxes(prominent peaks were found in the morning of October and in the afternoon of April,respectively).The highest diurnal variation in the N_2O fluxes took place at 15:00(86.4 μg N_2O m^(–2) h^(–1)) in June with an unimodal distribution.Water logging in October increased the emission of CO_2(especially at nighttime),yet decreased N_2O and CH_4 emissions to a different degree on the daily scale because of the restrained diffusion rates of the gases.The seasonal and diurnal variations of CH_4 and CO_2 fluxes did not correlate to the air and soil temperatures,whereas the seasonal and diurnal variation of the fluxes of N_2O in June exhibited a significant correlation with air temperature.When N_2O and CH_4 fluxes were converted to CO_2-e equivalents,the emissions of N_2O had a remarkable potential to impact the global warming.The mean daily flux(MF) and total daily flux(TDF) were higher in the growing season,nevertheless,the MF and TDF of CO_2 were higher in October and those of CH_4 and N_2O were higher in June.In spite of the difference in the optimal sampling times throughout the observation period,our results obtained have implications for sampling and scaling strategies in estimating the GHG fluxes in coastal saline wetlands.
基金supported by the National High Technology Research and Development Program of China(863 Program)(No.2012AA03A611)
文摘Poly(amide-6-b-ethylene oxide)(Pebax1657)/1-butyl-3-methylimidazo-lium bis[trifluoromethyl)sulfonyl]-imide([Bmim][Tf2N]) blend membranes with different [Bmim][Tf2N] contents were prepared via solution casting and solvent evaporation method. The permeation properties of the blend membranes for CO2, N2,CH4 and H2 were studied, and the physical properties were characterized by differential scanning calorimeter(DSC) and X-ray diffraction(XRD). Results showed that [Bmim][Tf2N] was dispersed as amorphous phase in the blend membranes, which caused the decrease of Tg(PE) and crystallinity(PA). With the addition of [Bmim][Tf2N], the CO2 permeability increased and reached up to approximately 286 Barrer at 40 wt%[Bmim][Tf2N], which was nearly double that of pristine Pebax1657 membrane. The increase of CO2 permeability may be attributed to high intrinsic permeability of [Bmim][Tf2N], the increase of fractional free of volume(FFV) and plasticization effect. However, the CO2 permeability reduced firstly when the [Bmim][Tf2N]content was below 10 wt%, which may be due to that the small ions of [Bmim][Tf2N] in the gap of polymer chain inhibited the flexibility of polymer chain; the interaction between Pebax1657 and [Bmim][Tf2N]decreased the content of EO units available for CO2 transport and led to a more compact structure. For Pebax1657/[Bmim][Tf2N] blend membranes, the permeabilities of N2, H2 and CH4decreased with the increase of feed pressure due to the hydrostatic pressure effect, while CO2 permeability increased with the increase of feed pressure for that the CO2-induced plasticization effect was stronger than hydrostatic pressure effect.
文摘Graphene oxide (GO)-multiwalled carbon nanotube (MWCNT) composite was synthesized and characterized by X-ray diffraction, atomic force microscopy, scanning electron microscopy, micro Raman, Fourier transform infrared and ultraviolet-visible near infrared spectroscopy techniques. Spectral characteris- tics of cladding modified fiber optic gas sensors were studied for various concentrations of ammonia, ethanol and methanol at 27 ℃. Thickness of the gas sensing layer was controlled by varying the concentration of composite in ethanol medium (0.5 and 1 mg/mL) for three times dipping process. The O.S mg/ mL concentrated GO-MWCNT coated sensor showed 1.20, 1.40 and 1.15 times higher sensitivity than the GO coated sensor for ammonia, ethanol and methanol vapors, respectively. Furthermore, it exhibited 1.50, 1.80 and 1.80 times better sensitivity than 1 mg/mL concentrated GO-MWCNT coated sensor for ammonia, ethanol and methanol vapors, respectively. The presence of functional groups in GO increased the sen- sitivity. This is mainly attributed to the effective electron charge transfer between the composite materials and analytes.
文摘The collection of different cations in the A and B sites of ABO3 was explored for the regularity of perovskites phase formability.Here,Sr2?,La3?,and Ce4?are selected as the cations of site A.The site B is considered to be Mn or Co cations.XRD analysis and Fourier transform infrared spectroscopy results confirm the formation of perovskite structure for catalysts in which La3?and Sr2?are considered as the cations of site A.Ceria is detected as the main crystalline phase when Ce4?is selected to be cation of site A.It is found that the octahedral factor(rB/rO) takes the same important role as the tolerance factor to form cubic perovskite.Average crystallite size of the products was calculated by data of the XRD and measured by the TEM analysis.Results of the XRD and TEM studies were supported by the study of the particles size distribution,which was carried out in a particle size analyzer.The perovskite samples were also used for stoichiometric oxidation of carbon monoxide with air.
基金supported by the National Natural Science Foundation of China(Nos.22025604 and 22276204)the National Key R&D Program of China(Nos.2023YFC3708401 and 2022YFC3800404).
文摘To develop efficient catalysts for ambient carbon monoxide(CO)oxidation is significant for indoor air purification and also for many industrial applications.In this work,the catalytic activity for CO oxidation were enhanced by tuning the metal-support interaction of Ru/CeO_(2)catalysts.A series of Ru/CeO_(2)catalysts were synthesized by an impregnation method with calcination at 100,200,400 and 600℃,respectively,to regulate the Ru-CeO_(2)interaction.We discovered that low temperature calcination(100℃)induced more Ru-O-Ce bonds and stronger Ru-CeO_(2)interaction,while high temperature calcination(≥400℃)caused the agglomeration of Ru species with more Ru-O-Ru bonds and weaker Ru-CeO_(2)interaction,resulting in the lower redox capacity of these catalysts,as well as lower catalytic activity for CO oxidation.Only calcination at moderate 200℃ can induce the moderate interaction between Ru species and CeO_(2)support,which can keep the high dispersion of RuO_(x)species with the high redox capacity,thus leading to complete elimination of 500 ppm CO at room temperature on Ru/Ce-200 catalyst.
文摘Pd/C catalysts were prepared by deposited Pd nanoparticles (NPs) on different carbon supports including activated carbon (AC), graphite oxide (GO), and reduced graphite oxide (rGO) using sol-immobilization method. Through transmission electron microscopy, powder X-ray di raction, and X-ray photoelectron spectroscopy, the role of the carbon supports for the catalytic performances of Pd/C catalysts was examined in selective hydrogenation of acetylene. The results indicate that Pd/AC exhibited higher activity and selectivity than Pd/GO and Pd/rGO in the gas phase selective hydrogenation of acetylene. Thermal and chemical treatment of AC supports also have some effect on the catalytic performance of Pd/AC catalysts. The differences in the activity and selectivity of various Pd/C catalysts were partly attributed to the metal-support interaction.
基金supported by the National Natural Science Foundation of China (21373259, 21301107)the Hundred Talents Project of the Chinese Academy of Sciences, the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA09030102)+2 种基金the Open Funding from Key Laboratory of Interfacial Physics and Technology, Chinese Academy of Sciencesthe Fundamental Research Fund-ing of Shandong University (2014JC005)the Taishan Scholar Project of Shandong Province (China)~~
文摘Nanostructured gold catalyst supported on metal oxide is highly active for the CO oxidation reac‐tion. In this work, a new type of oxide support, zinc tin oxide, has been used to deposit 0.7 wt%Au via a deposition‐precipitation method. The textural properties of Zn2SnO4 support have been tuned by varying the molar ratio between base (N2H4·H2O) and metal ion (Zn2+) to be 4/1, 8/1 and 16/1. The catalytic tests for CO oxidation reaction revealed that the reactivity on Au‐Zn2SnO4 with N2H4·H2O/Zn2+ = 8/1 was the highest, while the reactivity on Au‐Zn2SnO4 with N2H4·H2O/Zn2+ =16/1 was almost identical to that of the pure support. Both fresh and used catalysts have been characterized by multiple techniques including nitrogen adsorption‐desorption, X‐ray diffraction, transmission electron microscopy, high‐angle annular dark‐field scanning transmission electron microscopy, X‐ray photoelectron spectroscopy, X‐ray adsorption fine structure, and tempera‐ture‐programmed reduction by hydrogen. These demonstrated that the textural properties, espe‐cially pore volume and pore size distribution, of Zn2SnO4 play crucial roles in the averaged size of gold nanoparticles, and thus determine the catalytic activity of Au‐Zn2SnO4 for CO oxidation.