A SiC/ZrSiO4？SiO2 （SZS） coating was successfully fabricated on the carbon/carbon （C/C） composites by pack cementation, slurry painting and sintering to improve the anti-oxidation property and thermal shock r...A SiC/ZrSiO4？SiO2 （SZS） coating was successfully fabricated on the carbon/carbon （C/C） composites by pack cementation, slurry painting and sintering to improve the anti-oxidation property and thermal shock resistance. The anti-oxidation properties under different oxygen partial pressures （OPP） and thermal shock resistance of the SZS coating were investigated. The results show that the SZS coated sample under low OPP, corresponding to the ambient air, during isothermal oxidation was 0.54% in mass gain after 111 h oxidation at 1500 ° C and less than 0.03% in mass loss after 50 h oxidation in high OPP, corresponding to the air flow rate of 36 L/h. Additionally, the residual compressive strengths （RCS） of the SZS coated samples after oxidation for 50 h in high OPP and 80 h in low OPP remain about 70% and 72.5% of those of original C/C samples, respectively. Moreover, the mass loss of SZS coated samples subjected to the thermal cycle from 1500 ° C in high OPP to boiling water for 30 times was merely 1.61%.展开更多
BNp/Al2O3-SiO2 system ceramic matrix composites with different volume fractions （10%-60%） of hexagonal BN particulates （BNp） were prepared by hot-press sintering technique. Phase components, microstructure, mechan...BNp/Al2O3-SiO2 system ceramic matrix composites with different volume fractions （10%-60%） of hexagonal BN particulates （BNp） were prepared by hot-press sintering technique. Phase components, microstructure, mechanical properties and plasma erosion resistance were also investigated. With the increase of h-BNp content, relative density and Vickers＇ hardness of the composite ceramics decrease, while the flexural strength, elastic modulus and fracture toughness increase and then decrease. The plasma erosion resistance linearly deteriorated with the increase of BNp content which is mainly determined by the density, crystal structure and atomic number of the elements.展开更多
The utilization of metal oxide‐zeolite catalysts in the syngas‐to‐olefin reaction is a promising strategy for producing C_(2)–C_(4) olefins from non‐petroleum resources.However,the effect of the crystal phase of ...The utilization of metal oxide‐zeolite catalysts in the syngas‐to‐olefin reaction is a promising strategy for producing C_(2)–C_(4) olefins from non‐petroleum resources.However,the effect of the crystal phase of metal oxides on the catalytic activity of these oxides is still ambiguous.Herein,typical metal oxides(ZnO/ZrO_(2))with different crystal phases(monoclinic(m‐ZrO_(2))and tetragonal(t‐ZrO_(2)))were employed for syngas conversion.The(ZnO/m‐ZrO_(2)+SAPO‐34)composite catalyst exhibited 80.5%selectivity for C_(2)–C_(4) olefins at a CO conversion of 27.9%,where the results are superior to those(CO conversion of 16.4%and C_(2)–C_(4) olefin selectivity of 76.1%)obtained over(ZnO/t‐ZrO_(2)+SAPO‐34).The distinct differences are ascribed to the larger number of hydroxyl groups,Lewis acid sites,and oxygen defects in ZnO/m‐ZrO_(2) compared to ZnO/t‐ZrO_(2).These features result in the formation of more formate and methoxy intermediate species on the ZnO/m‐ZrO_(2) oxides during syngas conversion,followed by the formation of more light olefins over SAPO‐34.The present findings provide useful information for the design of highly efficient ZrO_(2)‐based catalysts for syngas conversion.展开更多
This article reports the production of COx free hydrogen and carbon nanofibers by the catalytic decomposition of methane over Ni-Al2O3-SiO2 catalysts. The influence of reaction temperature, pretreatment temperature, a...This article reports the production of COx free hydrogen and carbon nanofibers by the catalytic decomposition of methane over Ni-Al2O3-SiO2 catalysts. The influence of reaction temperature, pretreatment temperature, and effect of reductive pretreatment on the decomposition of methane activity is investigated. The physico-chemical characteristics of fresh and deactivated samples were characterized using BET-SA, XRD, TPR, SEM/TEM, CHNS analyses and correlated with the methane decomposition results obtained. The Ni-Al-Si （4 ： 0.5 ： 1.5） catalyst reduced with hydrazine hydrate produced better H2 yields of ca. 1815 mol H2/mol Ni than the catalyst reduced with 5% H2/N2.展开更多
Al 2O 3-SiO 2-TiO 2-ZrO 2 supported membranes were prepar ed by Sol-Gel method. These composite ceramic membranes are level, even and no macro crack. There exist several crystalline phases such as Al 2O 3, TiO...Al 2O 3-SiO 2-TiO 2-ZrO 2 supported membranes were prepar ed by Sol-Gel method. These composite ceramic membranes are level, even and no macro crack. There exist several crystalline phases such as Al 2O 3, TiO 2(a natase), Al 2SiO 5, and ZrO 2 in these membranes. Changing the molar ratio of Al∶Si∶Ti∶Zr,the kinds and content of crystal phases of composite membranes could be different, which may lead to a variety of microstructure of membranes. The surface nanoscale topography and microstructure of membranes were investiga ted by XRD,SEM,AFM,EPMA. The effects of additives and heat treatments on the sur face nanoscale topography and microstructure of composite ceramic membranes were also analyzed.展开更多
TiO2-coated activated carbon surface （TAs） composites were prepared by a sol-gel method with supercritical pretreatment. The photocatalytic degradation of acid yellow （AY） was investigated under UV radiation to es...TiO2-coated activated carbon surface （TAs） composites were prepared by a sol-gel method with supercritical pretreatment. The photocatalytic degradation of acid yellow （AY） was investigated under UV radiation to estimate activity of catalysts and determine the kinetics. And the effects of parameters including the initial concentration of AY, light intensity and TiO2 content in catalysts were examined. The results indicate that TAs has a higher efficiency in decomposition of AY than P25, pure TiO2 particles as well as the mixture of TiO2 powder and active carbon. The photocatalytic degradation rate is found to follow the pseudo-first order kinetics with respect to the AY concentration. The new kinetic model fairly resembles the classic Langmuir-Hinshelwood equation, and the rate constant is proportional to the square root of the light intensity in a wide range. However, its absorption performance depends on the surface areas of catalysts. The model fits quite well with the experimental data and elucidates phenomena about the effects of the TiO2 content in TAs on the degradation rate.展开更多
A series of polymer- supported Pd -Fe2O3 composite catalysts were prepared and their hydrogenation property mas investigated. It was found that the above catalysts have good catalytic hydrogenation activity for carbon...A series of polymer- supported Pd -Fe2O3 composite catalysts were prepared and their hydrogenation property mas investigated. It was found that the above catalysts have good catalytic hydrogenation activity for carbon - carbon double bonds systems and reusability. Furthermore, XPS and IR spectra shouted that active component in the composite catalysts is atomic Pd(0). An addition of a small amount of Fe2O3 has a promotive action upon hydrogenation activity of the catalysts, which indicated that there are some strong interactions (electron transfer) between Pd(0) and Fe(Ⅲ) species. Based on these results, a possible catalytic hydrogenation mechanism was also suggested.展开更多
Owing to outstanding hydrophilicity and ionic interaction,layered double hydroxides(LDHs)have emerged as a promising carrier for high performance catalysts.However,the synthesis of new specialized catalytic LDHs for d...Owing to outstanding hydrophilicity and ionic interaction,layered double hydroxides(LDHs)have emerged as a promising carrier for high performance catalysts.However,the synthesis of new specialized catalytic LDHs for degradation of antibiotics still faces some challenges.In this study,a CoFe_(2)O_(4)/MgAl-LDH composite catalyst was synthesized using a hydrothermal coprecipitation method.Comprehensive characterization reveals that the surface of MgAl-LDH is covered with nanometer CoFe_(2)O_(4) particles.The specific surface area of CoFe_(2)O_(4)/MgAl-LDH is 82.84 m^(2)·g^(-)1,which is 2.34 times that of CoFe_(2)O_(4).CoFe_(2)O_(4)/MgAl-LDH has a saturation magnetic strength of 22.24 A·m^(2)·kg^(-1) facilitating efficient solid-liquid separation.The composite catalyst was employed to activate peroxymonosulfate(PMS)for the efficient degradation of tetracycline hydrochloride(TCH).It is found that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH significantly exceeds that of CoFe_(2)O_(4).The maximum TCH removal reaches 98.2%under the optimal conditions([TCH]=25 mg/L,[PMS]=1.5 mmol/L,CoFe_(2)O_(4)/MgAl-LDH=0.20 g/L,pH 7,and T=25℃).Coexisting ions in the solution,such as SO_(4)^(2-),Cl-,H_(2)PO_(4)^(-),and CO_(3)^(2-),have a negligible effect on catalytic performance.Cyclic tests demonstrate that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH remains 67.2%after five cycles.Mechanism investigations suggest that O_(2)^(•-)and ^(1)O_(2) produced by CoFe_(2)O_(4)/MgAl-LDH play a critical role in the catalytic degradation.展开更多
A series of catalysts were prepared by doping different loadings of CeO2 over TiO2-SiO2-WO3 and used for the selective catalytic reduction of NOx by NH3. The experimental results showed that the selective catalytic re...A series of catalysts were prepared by doping different loadings of CeO2 over TiO2-SiO2-WO3 and used for the selective catalytic reduction of NOx by NH3. The experimental results showed that the selective catalytic reduction（SCR） performance and SO2-resistant ability of TiO2-SiO2-WO3 were greatly enhanced by the introduction of cerium. The catalyst containing 10% CeO2 showed the highest NO conversion in a wide temperature range and good N2 selectivity with broad operation temperature window at the gas hourly space velocity（GHSV） of 30000 h–1, which was a very promising catalyst for NOx abatement from diesel engine exhaust. The catalysts were characterized by X-ray diffraction（XRD）, scanning electron microscopy with energy dispersive X-ray spectroscopy（SEM-EDS）, N2 adsorption-desorption（BET） and X-ray photoelectron spectroscopy（XPS）. The characterization results showed that the bigger pore radius, higher surface atomic concentration and dispersion of Ce and the abundant adsorbed oxygen on the surface of catalyst contributed to the best NH3-SCR performance of CeO2/TiO2-SiO2-WO3 catalyst containing 10% CeO2.展开更多
In this work,syngas methanation over Ni-W/TiO2-SiO2catalyst was studied in a fluidized-bed reactor(FBR)and its performance was compared with a fixed-bed reactor(FIXBR).The effects of main operating variables including...In this work,syngas methanation over Ni-W/TiO2-SiO2catalyst was studied in a fluidized-bed reactor(FBR)and its performance was compared with a fixed-bed reactor(FIXBR).The effects of main operating variables including feedstock gases space velocity,coke content,bed temperature and sulfur-tolerant stability of 100 h life were investigated.The structure of the catalysts was characterized by XRD,N2adsorptiondesorption and TEM.It is found that under same space velocity from 5000 h 1to 25000 h 1FBR gave a higher CH4yield,lower coke content,and lower bed temperature than those obtained in FIXBR.Ni-W/TiO2-SiO2catalyst possessed excellent sulfur-tolerant stability on the feedstock gases less than 500 ppm H2S in FBR.The carbon deposits formed on the spent catalyst were in the form of carbon fibers in FBR,while in the form of dense accumulation distribution appearance in FIXBR.展开更多
An efficient and direct procedure has been developed for the preparation of amidoalkyl naphthols by a one-pot condensation of aryl aldehydes, 2-naphthol and urea or amides, in the presence of HClO4-SiO2 as a heterogen...An efficient and direct procedure has been developed for the preparation of amidoalkyl naphthols by a one-pot condensation of aryl aldehydes, 2-naphthol and urea or amides, in the presence of HClO4-SiO2 as a heterogeneous catalyst. The reactions were carried out under reflux and solvent-free conditions. The present methodology offers several advantages such as excellent yields, simple procedure, easy work-up and ecofriendly reaction condition. The catalyst is easily prepared, stable, reusable and efficient under the reaction conditions.展开更多
The influence of calcination temperature on the structure and catalytic behavior of Ni/TiO2-SiO2 catalyst, for CO2 reforming of methane to synthesis gas under atmospheric pressure, was investigated. The results showed...The influence of calcination temperature on the structure and catalytic behavior of Ni/TiO2-SiO2 catalyst, for CO2 reforming of methane to synthesis gas under atmospheric pressure, was investigated. The results showed that the Ni/TiO2-SiO2 catalyst calcined at 700 ℃ had high and stable activity while the catalysts calcined at 550 and 850 ℃ had low and unstable activity. Depending on the calcination temperature, one, two, or three of the following Ni-containing species, NiO, Ni2.44Ti0.72Si0.07O4, and NiTiO3 were identified by combining the temperature programmed reduction （TPR） and X-ray diffraction （XRD） results. Their reducibility decreased in the sequence： NiO〉Ni2.44Ti0.72Si0.07O4〉NiTiO3. It suggests that high and stable activities observed over the Ni/TiO2-SiO2 catalyst calcined at 700 ~C were induced by the formation of Ni2.44Ti0.72Si0.07O4 and smaller NiO species crystallite size.展开更多
Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by...Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by a series of characterization techniques including BET, XRD, SEM, EDX-mapping, TEM, H_2-TPR, XPS, NH_3-TPD and Py-FTIR. Compared to Ni/Al_2O_3 catalyst, the SiO_2-doped samples exhibited better B_3D conversion. SiO_2 could help to form a strong interaction between NiO with the support, which inhibited Ni agglomeration at high temperature, improved the Ni dispersion, and enhanced the hydrogenation activity. B_1D selectivity was mainly influenced by the quantity of Lewis acid sites in addition to the Ni dispersion. The catalyst with a silica loading of 6.4% demonstrated an excellent selectivity of 75.18%(by 13% higher than the contrastive Ni/Al_2O_3 catalyst), which was attributed to the larger amount of Lewis acid sites and the moderate interaction between NiO with the support, which could facilitate the nickel dispersion on a preferable surface area of 176.3 m^2/g of support.展开更多
Transition metal Ni anchored in carbon material represents outstanding 2e^(-) oxygen reduction reaction(ORR)catalytic selectivity,but enhancing the adsorption strength of intermediate*OOH to promote its selectivity re...Transition metal Ni anchored in carbon material represents outstanding 2e^(-) oxygen reduction reaction(ORR)catalytic selectivity,but enhancing the adsorption strength of intermediate*OOH to promote its selectivity remains a major challenge.Herein,the NiX/Ni@NCHS composite catalyst with heteroatom doping(O,S)is modulated by controlling partial pyrolysis strategies on honeycomb-like porous carbon to manipulate the electronic structure of the metal Ni.With the synergistic effect of honeycomb structure and O atom,NiO/Ni@NCHS-700 exhibits an exceptional H_(2)O_(2)selectivity of above 89.1%across a wide potential range from 0.1 to 0.6 V in an alkaline electrolyte,and an unexpected H_(2)O_(2)production rate up to 1.47 mol gcat^(-1) h^(-1)@0.2 V,which outperforms most of the state-of-the-art catalyst.Meanwhile,NiS/Ni@NCHS exhibits excellent electrocatalytic performance,with 2e^(-) ORR selectivity of 91.3%,H_(2)O_(2)yield of 1.85@0.3 V.Density functional theory simulations and experiments results reveal that the heteroatom doping(O,S)method has been employed to regulate the adsorption strength of Ni atoms with*OOH,and combined with the self-sacrificing template-assisted pyrolysis approach to improve the microstructure of catalysts and optimize the active site.The heteroatom doping method in this work provides significant guidance for promoting 2e^(-) ORR electrocatalysis to produce H_(2)O_(2).展开更多
Mg2Ni0.8Cr0.2-x wt.% CoO/Al2O3 (x=0.5, 1, 2 and 3) composites were prepared by mechanically milling sintered Mg2Ni0.8Cr0.2 alloy and CoO/Al2O3 compound for 45 h. The addition of CoO/Al2O3 compound resulted in the good...Mg2Ni0.8Cr0.2-x wt.% CoO/Al2O3 (x=0.5, 1, 2 and 3) composites were prepared by mechanically milling sintered Mg2Ni0.8Cr0.2 alloy and CoO/Al2O3 compound for 45 h. The addition of CoO/Al2O3 compound resulted in the good kinetics properties of hydriding/dehydriding reaction of the composites. The composite with 1.0 wt.% CoO/Al2O3 catalyst could reach the maximum hydrogen absorption capacity (2.9 wt.%) within 5 min at 393 K under H2 pressure of 4 MPa, and can desorb rapidly at 493 K. The decomposition and synthesis of hydrogen molecule on Mg2Ni0.8Cr0.2 alloy surface was promoted by addition of CoO/Al2O3 catalyst. In addition, the formation of metallic Ni particles, strain and defects during the ball milling process also resulted in the improved hydrogenation performance of Mg2Ni-based alloys.展开更多
基金Project supported by the Nonferrous Metal Oriented Advanced Structural Materials and Manufacturing Cooperative Innovation Center,ChinaProject(51205417)supported by the National Natural Science Foundation of China
文摘A SiC/ZrSiO4？SiO2 （SZS） coating was successfully fabricated on the carbon/carbon （C/C） composites by pack cementation, slurry painting and sintering to improve the anti-oxidation property and thermal shock resistance. The anti-oxidation properties under different oxygen partial pressures （OPP） and thermal shock resistance of the SZS coating were investigated. The results show that the SZS coated sample under low OPP, corresponding to the ambient air, during isothermal oxidation was 0.54% in mass gain after 111 h oxidation at 1500 ° C and less than 0.03% in mass loss after 50 h oxidation in high OPP, corresponding to the air flow rate of 36 L/h. Additionally, the residual compressive strengths （RCS） of the SZS coated samples after oxidation for 50 h in high OPP and 80 h in low OPP remain about 70% and 72.5% of those of original C/C samples, respectively. Moreover, the mass loss of SZS coated samples subjected to the thermal cycle from 1500 ° C in high OPP to boiling water for 30 times was merely 1.61%.
基金Project(HIT.NSRIF.2010112)supported by the Fundamental Research Fund for the Central Universities,ChinaProjects(50902030,51021002)supported by the National Natural Science Foundation of China
文摘BNp/Al2O3-SiO2 system ceramic matrix composites with different volume fractions （10%-60%） of hexagonal BN particulates （BNp） were prepared by hot-press sintering technique. Phase components, microstructure, mechanical properties and plasma erosion resistance were also investigated. With the increase of h-BNp content, relative density and Vickers＇ hardness of the composite ceramics decrease, while the flexural strength, elastic modulus and fracture toughness increase and then decrease. The plasma erosion resistance linearly deteriorated with the increase of BNp content which is mainly determined by the density, crystal structure and atomic number of the elements.
文摘The utilization of metal oxide‐zeolite catalysts in the syngas‐to‐olefin reaction is a promising strategy for producing C_(2)–C_(4) olefins from non‐petroleum resources.However,the effect of the crystal phase of metal oxides on the catalytic activity of these oxides is still ambiguous.Herein,typical metal oxides(ZnO/ZrO_(2))with different crystal phases(monoclinic(m‐ZrO_(2))and tetragonal(t‐ZrO_(2)))were employed for syngas conversion.The(ZnO/m‐ZrO_(2)+SAPO‐34)composite catalyst exhibited 80.5%selectivity for C_(2)–C_(4) olefins at a CO conversion of 27.9%,where the results are superior to those(CO conversion of 16.4%and C_(2)–C_(4) olefin selectivity of 76.1%)obtained over(ZnO/t‐ZrO_(2)+SAPO‐34).The distinct differences are ascribed to the larger number of hydroxyl groups,Lewis acid sites,and oxygen defects in ZnO/m‐ZrO_(2) compared to ZnO/t‐ZrO_(2).These features result in the formation of more formate and methoxy intermediate species on the ZnO/m‐ZrO_(2) oxides during syngas conversion,followed by the formation of more light olefins over SAPO‐34.The present findings provide useful information for the design of highly efficient ZrO_(2)‐based catalysts for syngas conversion.
文摘This article reports the production of COx free hydrogen and carbon nanofibers by the catalytic decomposition of methane over Ni-Al2O3-SiO2 catalysts. The influence of reaction temperature, pretreatment temperature, and effect of reductive pretreatment on the decomposition of methane activity is investigated. The physico-chemical characteristics of fresh and deactivated samples were characterized using BET-SA, XRD, TPR, SEM/TEM, CHNS analyses and correlated with the methane decomposition results obtained. The Ni-Al-Si （4 ： 0.5 ： 1.5） catalyst reduced with hydrazine hydrate produced better H2 yields of ca. 1815 mol H2/mol Ni than the catalyst reduced with 5% H2/N2.
文摘Al 2O 3-SiO 2-TiO 2-ZrO 2 supported membranes were prepar ed by Sol-Gel method. These composite ceramic membranes are level, even and no macro crack. There exist several crystalline phases such as Al 2O 3, TiO 2(a natase), Al 2SiO 5, and ZrO 2 in these membranes. Changing the molar ratio of Al∶Si∶Ti∶Zr,the kinds and content of crystal phases of composite membranes could be different, which may lead to a variety of microstructure of membranes. The surface nanoscale topography and microstructure of membranes were investiga ted by XRD,SEM,AFM,EPMA. The effects of additives and heat treatments on the sur face nanoscale topography and microstructure of composite ceramic membranes were also analyzed.
基金Project(50802034) supported by the National Natural Science Foundation of ChinaProject(11A093) supported by the Key Project Foundation by the Education Department of Hunan Province,China
文摘TiO2-coated activated carbon surface （TAs） composites were prepared by a sol-gel method with supercritical pretreatment. The photocatalytic degradation of acid yellow （AY） was investigated under UV radiation to estimate activity of catalysts and determine the kinetics. And the effects of parameters including the initial concentration of AY, light intensity and TiO2 content in catalysts were examined. The results indicate that TAs has a higher efficiency in decomposition of AY than P25, pure TiO2 particles as well as the mixture of TiO2 powder and active carbon. The photocatalytic degradation rate is found to follow the pseudo-first order kinetics with respect to the AY concentration. The new kinetic model fairly resembles the classic Langmuir-Hinshelwood equation, and the rate constant is proportional to the square root of the light intensity in a wide range. However, its absorption performance depends on the surface areas of catalysts. The model fits quite well with the experimental data and elucidates phenomena about the effects of the TiO2 content in TAs on the degradation rate.
文摘A series of polymer- supported Pd -Fe2O3 composite catalysts were prepared and their hydrogenation property mas investigated. It was found that the above catalysts have good catalytic hydrogenation activity for carbon - carbon double bonds systems and reusability. Furthermore, XPS and IR spectra shouted that active component in the composite catalysts is atomic Pd(0). An addition of a small amount of Fe2O3 has a promotive action upon hydrogenation activity of the catalysts, which indicated that there are some strong interactions (electron transfer) between Pd(0) and Fe(Ⅲ) species. Based on these results, a possible catalytic hydrogenation mechanism was also suggested.
基金University Synergy Innovation Program of Anhui Province(GXXT-2022-083)Science and Technology Plan Project of Wuhu City,China(2023kx12)Anhui Provincial Department of Education New Era Education Project(2023xscx070)。
文摘Owing to outstanding hydrophilicity and ionic interaction,layered double hydroxides(LDHs)have emerged as a promising carrier for high performance catalysts.However,the synthesis of new specialized catalytic LDHs for degradation of antibiotics still faces some challenges.In this study,a CoFe_(2)O_(4)/MgAl-LDH composite catalyst was synthesized using a hydrothermal coprecipitation method.Comprehensive characterization reveals that the surface of MgAl-LDH is covered with nanometer CoFe_(2)O_(4) particles.The specific surface area of CoFe_(2)O_(4)/MgAl-LDH is 82.84 m^(2)·g^(-)1,which is 2.34 times that of CoFe_(2)O_(4).CoFe_(2)O_(4)/MgAl-LDH has a saturation magnetic strength of 22.24 A·m^(2)·kg^(-1) facilitating efficient solid-liquid separation.The composite catalyst was employed to activate peroxymonosulfate(PMS)for the efficient degradation of tetracycline hydrochloride(TCH).It is found that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH significantly exceeds that of CoFe_(2)O_(4).The maximum TCH removal reaches 98.2%under the optimal conditions([TCH]=25 mg/L,[PMS]=1.5 mmol/L,CoFe_(2)O_(4)/MgAl-LDH=0.20 g/L,pH 7,and T=25℃).Coexisting ions in the solution,such as SO_(4)^(2-),Cl-,H_(2)PO_(4)^(-),and CO_(3)^(2-),have a negligible effect on catalytic performance.Cyclic tests demonstrate that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH remains 67.2%after five cycles.Mechanism investigations suggest that O_(2)^(•-)and ^(1)O_(2) produced by CoFe_(2)O_(4)/MgAl-LDH play a critical role in the catalytic degradation.
基金supported by the National Natural Science Foundation of China(21173153)the National High Technology Research and Development Program of China(863 project)(2013AA065304)
文摘A series of catalysts were prepared by doping different loadings of CeO2 over TiO2-SiO2-WO3 and used for the selective catalytic reduction of NOx by NH3. The experimental results showed that the selective catalytic reduction（SCR） performance and SO2-resistant ability of TiO2-SiO2-WO3 were greatly enhanced by the introduction of cerium. The catalyst containing 10% CeO2 showed the highest NO conversion in a wide temperature range and good N2 selectivity with broad operation temperature window at the gas hourly space velocity（GHSV） of 30000 h–1, which was a very promising catalyst for NOx abatement from diesel engine exhaust. The catalysts were characterized by X-ray diffraction（XRD）, scanning electron microscopy with energy dispersive X-ray spectroscopy（SEM-EDS）, N2 adsorption-desorption（BET） and X-ray photoelectron spectroscopy（XPS）. The characterization results showed that the bigger pore radius, higher surface atomic concentration and dispersion of Ce and the abundant adsorbed oxygen on the surface of catalyst contributed to the best NH3-SCR performance of CeO2/TiO2-SiO2-WO3 catalyst containing 10% CeO2.
文摘In this work,syngas methanation over Ni-W/TiO2-SiO2catalyst was studied in a fluidized-bed reactor(FBR)and its performance was compared with a fixed-bed reactor(FIXBR).The effects of main operating variables including feedstock gases space velocity,coke content,bed temperature and sulfur-tolerant stability of 100 h life were investigated.The structure of the catalysts was characterized by XRD,N2adsorptiondesorption and TEM.It is found that under same space velocity from 5000 h 1to 25000 h 1FBR gave a higher CH4yield,lower coke content,and lower bed temperature than those obtained in FIXBR.Ni-W/TiO2-SiO2catalyst possessed excellent sulfur-tolerant stability on the feedstock gases less than 500 ppm H2S in FBR.The carbon deposits formed on the spent catalyst were in the form of carbon fibers in FBR,while in the form of dense accumulation distribution appearance in FIXBR.
文摘An efficient and direct procedure has been developed for the preparation of amidoalkyl naphthols by a one-pot condensation of aryl aldehydes, 2-naphthol and urea or amides, in the presence of HClO4-SiO2 as a heterogeneous catalyst. The reactions were carried out under reflux and solvent-free conditions. The present methodology offers several advantages such as excellent yields, simple procedure, easy work-up and ecofriendly reaction condition. The catalyst is easily prepared, stable, reusable and efficient under the reaction conditions.
文摘The influence of calcination temperature on the structure and catalytic behavior of Ni/TiO2-SiO2 catalyst, for CO2 reforming of methane to synthesis gas under atmospheric pressure, was investigated. The results showed that the Ni/TiO2-SiO2 catalyst calcined at 700 ℃ had high and stable activity while the catalysts calcined at 550 and 850 ℃ had low and unstable activity. Depending on the calcination temperature, one, two, or three of the following Ni-containing species, NiO, Ni2.44Ti0.72Si0.07O4, and NiTiO3 were identified by combining the temperature programmed reduction （TPR） and X-ray diffraction （XRD） results. Their reducibility decreased in the sequence： NiO〉Ni2.44Ti0.72Si0.07O4〉NiTiO3. It suggests that high and stable activities observed over the Ni/TiO2-SiO2 catalyst calcined at 700 ~C were induced by the formation of Ni2.44Ti0.72Si0.07O4 and smaller NiO species crystallite size.
基金Financial support from the National Natural Science Foundation of China (21163019) is gratefully acknowledged
文摘Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by a series of characterization techniques including BET, XRD, SEM, EDX-mapping, TEM, H_2-TPR, XPS, NH_3-TPD and Py-FTIR. Compared to Ni/Al_2O_3 catalyst, the SiO_2-doped samples exhibited better B_3D conversion. SiO_2 could help to form a strong interaction between NiO with the support, which inhibited Ni agglomeration at high temperature, improved the Ni dispersion, and enhanced the hydrogenation activity. B_1D selectivity was mainly influenced by the quantity of Lewis acid sites in addition to the Ni dispersion. The catalyst with a silica loading of 6.4% demonstrated an excellent selectivity of 75.18%(by 13% higher than the contrastive Ni/Al_2O_3 catalyst), which was attributed to the larger amount of Lewis acid sites and the moderate interaction between NiO with the support, which could facilitate the nickel dispersion on a preferable surface area of 176.3 m^2/g of support.
文摘Transition metal Ni anchored in carbon material represents outstanding 2e^(-) oxygen reduction reaction(ORR)catalytic selectivity,but enhancing the adsorption strength of intermediate*OOH to promote its selectivity remains a major challenge.Herein,the NiX/Ni@NCHS composite catalyst with heteroatom doping(O,S)is modulated by controlling partial pyrolysis strategies on honeycomb-like porous carbon to manipulate the electronic structure of the metal Ni.With the synergistic effect of honeycomb structure and O atom,NiO/Ni@NCHS-700 exhibits an exceptional H_(2)O_(2)selectivity of above 89.1%across a wide potential range from 0.1 to 0.6 V in an alkaline electrolyte,and an unexpected H_(2)O_(2)production rate up to 1.47 mol gcat^(-1) h^(-1)@0.2 V,which outperforms most of the state-of-the-art catalyst.Meanwhile,NiS/Ni@NCHS exhibits excellent electrocatalytic performance,with 2e^(-) ORR selectivity of 91.3%,H_(2)O_(2)yield of 1.85@0.3 V.Density functional theory simulations and experiments results reveal that the heteroatom doping(O,S)method has been employed to regulate the adsorption strength of Ni atoms with*OOH,and combined with the self-sacrificing template-assisted pyrolysis approach to improve the microstructure of catalysts and optimize the active site.The heteroatom doping method in this work provides significant guidance for promoting 2e^(-) ORR electrocatalysis to produce H_(2)O_(2).
基金Project (No. TG20000264-06) supported by the Special Funds forMajor States Basic Research Project of MOST, China
文摘Mg2Ni0.8Cr0.2-x wt.% CoO/Al2O3 (x=0.5, 1, 2 and 3) composites were prepared by mechanically milling sintered Mg2Ni0.8Cr0.2 alloy and CoO/Al2O3 compound for 45 h. The addition of CoO/Al2O3 compound resulted in the good kinetics properties of hydriding/dehydriding reaction of the composites. The composite with 1.0 wt.% CoO/Al2O3 catalyst could reach the maximum hydrogen absorption capacity (2.9 wt.%) within 5 min at 393 K under H2 pressure of 4 MPa, and can desorb rapidly at 493 K. The decomposition and synthesis of hydrogen molecule on Mg2Ni0.8Cr0.2 alloy surface was promoted by addition of CoO/Al2O3 catalyst. In addition, the formation of metallic Ni particles, strain and defects during the ball milling process also resulted in the improved hydrogenation performance of Mg2Ni-based alloys.
