Mesoporous Ni-Al composite oxide(MNA)with excellent textural and surface properties was prepared using a facile calcination-induced metal heteroatom doping approach and was evaluated as support of Pt-based catalyst fo...Mesoporous Ni-Al composite oxide(MNA)with excellent textural and surface properties was prepared using a facile calcination-induced metal heteroatom doping approach and was evaluated as support of Pt-based catalyst for methylcyclohexane dehydrogenation at a low temperature.The homogeneous incorporation of Ni atoms into the mesoporous framework of alumina and the formation of surface Ni-O-Al bonds benefit the generation of surface coordinated unsaturated aluminum species,which play a crucial role in highly homogenously dispersing Pt active sites in a form of single-atom clusters.Consequently,the resultant catalyst Pt/MNA displayed significantly improved catalytic performance.For example,at 300℃,catalyst Pt/MNA demonstrated a notable catalytic activity with a maximum hydrogen evolution rate of 3057 mmol/gPt/min,even after a long-time reaction up to 100 h or regeneration,which is inspiringly superior to the state-of-the-art supported Ptbased catalysts.The obviously boosted catalytic reactivity of catalyst Pt/MNA can be attributed to the excellent structural and textural properties,the remarkably raised Pt utilization efficiency,and the synergic catalytic effect derived from the interface electron transfer from support MNA to metallic Pt active sites.Our results provided a rational design strategy for the development of promising Pt-based catalyst for methylcyclohexane dehydrogenation,which is vital in the utilization of methylcyclohexane-toluene system for hydrogen storage.展开更多
Adsorption of pure CO_(2) and N2 and separation of CO_(2)/N2 mixture in MFI zeolite and MFI/MCM-41 micro/mesoporous composite have been studied by using atomistic simulations.Fully atomistic models of MFI and MFI/MCM-...Adsorption of pure CO_(2) and N2 and separation of CO_(2)/N2 mixture in MFI zeolite and MFI/MCM-41 micro/mesoporous composite have been studied by using atomistic simulations.Fully atomistic models of MFI and MFI/MCM-41 are constructed and characterized.A bimodal pore size distribution is observed in MFI/MCM-41 from simulated small-and broad-angle X-ray diffrac-tion patterns.The density of MFI/MCM-41 is lower than MFI,while its free volume and specific surface area are greater than MFI due to the presence of mesopores.CO_(2) is preferentially adsorbed than N2,and thus,the loading and isosteric heat of CO_(2) are greater than N2 in both MFI and MFI/MCM-41.CO_(2) isotherm in MFI/MCM-41 is similar to that in MFI at low pressures,but resembles that in MCM-41 at high pressures.N2 shows similar amount of loading in MFI,MCM-41 and MFI/MCM-41.The selectivity of CO_(2) over N2 in the three adsorbents decreases in the order of MFI>MFI/MCM-41>MCM-41.With increasing pressure,the selectivity increases in MFI and MFI/MCM-41,but decreases in MCM-41.The self-diffusivity of CO_(2) and N2 in MFI decreases as loading increases,while in MFI/MCM-41,itfirst increases and then drops.展开更多
A novel mesoporous HPMo/SiO2 composite was synthesized by the sol-gel method with triblock copolymer EO20PO70EO20 as template.The properties of the product were characterized by X-ray diffraction,transmission electron...A novel mesoporous HPMo/SiO2 composite was synthesized by the sol-gel method with triblock copolymer EO20PO70EO20 as template.The properties of the product were characterized by X-ray diffraction,transmission electron microscopy,N2 adsorption-desorption isotherms,Fourier transform infrared spectrometer and inductively-coupled plasma analysis.The experimental results show that the product has a very ordered hexagonal mesostructure,and the HPMo is immobilized into the framework of silica.The final mesoporous composite shows excellent stability in polar solvents.Results of catalytic tests indicate that the composite is an effective catalyst for oxidation of dibenzothiophen,and there are few activity losses even after the third cycle of uses.The high catalytic activity and good insolubility make it a promising catalyst in oxidative desulfurization process.展开更多
Mesoporous SiO2-ZrO7 nanocomposite was successfully prepared by using supramolecular tfiblock copolymer as the template through evaporation-induced self-assembly approach. The textural and structural properties were c...Mesoporous SiO2-ZrO7 nanocomposite was successfully prepared by using supramolecular tfiblock copolymer as the template through evaporation-induced self-assembly approach. The textural and structural properties were characterized by X-ray diffraction, nitrogen adsorption analysis, and transmission electron microscope. Comparison between pure mesoporous silica and mesoporous silica-zirconia nanocomposite was also presented in this work. The surface area, pore size, and pore volume decreased as the Zr doping in the mesoporous silica framework. But the obtained nanocomposite maintained the cubic Im3m-type mesoporous structure.展开更多
A mesoporous Al-Mg composite oxide with a hexagonal structure was synthesized with aluminium nitrate and magnesium nitrate as the reagents and sodium dodecyl sulfate（SDS） as the template in the presence of ethylened...A mesoporous Al-Mg composite oxide with a hexagonal structure was synthesized with aluminium nitrate and magnesium nitrate as the reagents and sodium dodecyl sulfate（SDS） as the template in the presence of ethylenediamine. The XRD, nitrogen adsorption-desorption and TEM studies indicate that the composite has a hexagonal framework structure and an average pore diameter of 2. 6 nm. The TG/DTA spectra indicate that the decomposition and the removal of the occluded surfactant of the sample take place in a range of 230-550 ℃. The mesoporous Al-Mg composite oxide exhibites a highly catalytic activity for the oxyethylation of fatty alcohols. Narrow-range distributed ethoxylates are formed in the presence of the mesoporous Al-Mg composite oxide catalyst. The distribution selectivity coefficient（Cx） is 24 when the mesoporous Al-Mg composite oxide was used as a catalyst for the oxyethylation of octanol and the average adduct degree of ethoxylates is 6. 4.展开更多
A novel mesoporous silica coated carbon composite(denoted SEG) with hierarchical pore structure has been successfully prepared in an aqueous solution that contains triblock copolymer template, aluminum chloride, silic...A novel mesoporous silica coated carbon composite(denoted SEG) with hierarchical pore structure has been successfully prepared in an aqueous solution that contains triblock copolymer template, aluminum chloride, siliceous source and expanded graphite. Textural property and morphology of the SEG composite were characterized by the combination of X-ray diffraction, N_2 adsorption–desorption, scanning electron microscopy,transmission electron microscopy and Fourier transform infrared measurements. Results show that mesoporous silica is steadily and uniformly grown on the surface of the graphite slices and the thickness of the silica layer can be finely tuned according to the silica/C molar ratio in the initial reaction solution. This newly synthesized SEG composite shows greatly increased adsorption capacity to methylene blue than the pristine expanded graphite in the batch tests. Both Langmuir and Frendlich models were further used to evaluate the adsorption isotherms of methylene blue over expanded graphite and SEG samples with different silica contents. Finally, pseudosecond-order model was used to describe the kinetics of methylene blue over expanded graphite and the silica-carbon composites.展开更多
Mesoporous CeO2-MnOx binary oxides with different Mn/Ce molar ratios were prepared by hydrothermal synthesis and characterized by scanning electron microscopy （SEM）, N2 sorption, X-ray diffraction （XRD）, X-ray pho...Mesoporous CeO2-MnOx binary oxides with different Mn/Ce molar ratios were prepared by hydrothermal synthesis and characterized by scanning electron microscopy （SEM）, N2 sorption, X-ray diffraction （XRD）, X-ray photoelectron spectroscopy （XPS） and H2 temperature-programmed reduction （H2-TPR）. The characterization results indicated that the CeO2-MnOx catalysts exhibited flower-like microspheres with high specific surface areas, and partial Mn cations could be incorporated into CeO2 lattice to form solid solution. The CeO2-MnOx catalysts showed better catalytic activity for CO oxidation than that prepared by the coprecipitation method. Furthermore, the CeO2-MnOx catalyst with Mn/Ce molar ratio of 1 in the synthesis gel （Ce-Mn-1） exhibited the best catalytic activity, over which the conversion of CO could achieve 90% at 135 ℃. This was ascribed to presence of more Mn species with higher oxida- tion state on the surface and the better reducibility over the Ce-Mn-I catalyst than other CeO2-MnOx catalysts.展开更多
A mesoporous LiFe0.99Mo0.01PO4/C composite was synthesized by the sol-gel method using （NH4）2MoO4 as a doping starting material. The formation of conductive carbon, metal doping and mesopores was achieved simultaneo...A mesoporous LiFe0.99Mo0.01PO4/C composite was synthesized by the sol-gel method using （NH4）2MoO4 as a doping starting material. The formation of conductive carbon, metal doping and mesopores was achieved simultaneously in the prepared material. The characterizations of crystal structures and microstructures were investigated using X-ray diffraction （XRD）, scanning electron microscopy （SEM）, transmission electron microscopy （TEM）, extended X-ray-absorption fine-structure （EXAFS） and X-ray-absorption near-structure spectroscopy （XANES） while the surface area was determined using N2 adsorption techniques. Cyclic voltammetry （CV） and charge-discharge cycling performance were used to characterize its electrochemical properties. The sample possessed uniformly distributed mesopores with an average pore size of 4 nm, and the specific surface area was about 69.368 m^2/g. The results show that the reversible capacity of mesoporous LiFe0.99Mo0.01PO4/C is about 160 mAh/g at 0.1C, 135 mAh/g at 1C and 90 mAh/g at 5C, respectively. The capacity fading is neglectable.展开更多
t In this paper,a facile strategy is proposed to controllably synthesize mesoporous Li_(4)Ti_(5)O_(12)/C nanocomposite embedded in graphene matrix as lithium-ion battery anode via the co-assembly of Li_(4)Ti_(5)O_(12)...t In this paper,a facile strategy is proposed to controllably synthesize mesoporous Li_(4)Ti_(5)O_(12)/C nanocomposite embedded in graphene matrix as lithium-ion battery anode via the co-assembly of Li_(4)Ti_(5)O_(12)(LTO)precursor,GO,and phenolic resin.The obtained composites,which consists of a LTO core,a phenolic-resin-based carbon shell,and a porous frame constructed by rGO,can be denoted as LTO/C/rGO and presents a hierarchical structure.Owing to the advantages of the hierarchical structure,including a high surface area and a high electric conductivity,the mesoporous LTO/C/rGO composite exhibits a greatly improved rate capability as the anode material in contrast to the conventional LTO electrode.展开更多
基金supported by the National Natural Science Foundation of China(21975174 and 22378286)the Natural Science Foundation of Shanxi Province,China(202403021221036)+1 种基金the Funds for Central Government to Guide Local Science and Technology Development(YDZJSX2021A014)the Research Project Supported by Shanxi Scholarship Council of China(2024-036).
文摘Mesoporous Ni-Al composite oxide(MNA)with excellent textural and surface properties was prepared using a facile calcination-induced metal heteroatom doping approach and was evaluated as support of Pt-based catalyst for methylcyclohexane dehydrogenation at a low temperature.The homogeneous incorporation of Ni atoms into the mesoporous framework of alumina and the formation of surface Ni-O-Al bonds benefit the generation of surface coordinated unsaturated aluminum species,which play a crucial role in highly homogenously dispersing Pt active sites in a form of single-atom clusters.Consequently,the resultant catalyst Pt/MNA displayed significantly improved catalytic performance.For example,at 300℃,catalyst Pt/MNA demonstrated a notable catalytic activity with a maximum hydrogen evolution rate of 3057 mmol/gPt/min,even after a long-time reaction up to 100 h or regeneration,which is inspiringly superior to the state-of-the-art supported Ptbased catalysts.The obviously boosted catalytic reactivity of catalyst Pt/MNA can be attributed to the excellent structural and textural properties,the remarkably raised Pt utilization efficiency,and the synergic catalytic effect derived from the interface electron transfer from support MNA to metallic Pt active sites.Our results provided a rational design strategy for the development of promising Pt-based catalyst for methylcyclohexane dehydrogenation,which is vital in the utilization of methylcyclohexane-toluene system for hydrogen storage.
基金supported by the National Natural Science Foundation of China(Grant Nos.20736002,20776045)the National High Technology Research and Development Program of China(No.2008AA062302)+1 种基金Program for Changjiang Scholars and Innovative Research Team in University of China(No.IRT0721)the 111 Project of China(No.B08021).
文摘Adsorption of pure CO_(2) and N2 and separation of CO_(2)/N2 mixture in MFI zeolite and MFI/MCM-41 micro/mesoporous composite have been studied by using atomistic simulations.Fully atomistic models of MFI and MFI/MCM-41 are constructed and characterized.A bimodal pore size distribution is observed in MFI/MCM-41 from simulated small-and broad-angle X-ray diffrac-tion patterns.The density of MFI/MCM-41 is lower than MFI,while its free volume and specific surface area are greater than MFI due to the presence of mesopores.CO_(2) is preferentially adsorbed than N2,and thus,the loading and isosteric heat of CO_(2) are greater than N2 in both MFI and MFI/MCM-41.CO_(2) isotherm in MFI/MCM-41 is similar to that in MFI at low pressures,but resembles that in MCM-41 at high pressures.N2 shows similar amount of loading in MFI,MCM-41 and MFI/MCM-41.The selectivity of CO_(2) over N2 in the three adsorbents decreases in the order of MFI>MFI/MCM-41>MCM-41.With increasing pressure,the selectivity increases in MFI and MFI/MCM-41,but decreases in MCM-41.The self-diffusivity of CO_(2) and N2 in MFI decreases as loading increases,while in MFI/MCM-41,itfirst increases and then drops.
基金Funded by the Hubei Provincial Department of Education Science and Technology Program for Outstanding Young Talents (Q20081209)
文摘A novel mesoporous HPMo/SiO2 composite was synthesized by the sol-gel method with triblock copolymer EO20PO70EO20 as template.The properties of the product were characterized by X-ray diffraction,transmission electron microscopy,N2 adsorption-desorption isotherms,Fourier transform infrared spectrometer and inductively-coupled plasma analysis.The experimental results show that the product has a very ordered hexagonal mesostructure,and the HPMo is immobilized into the framework of silica.The final mesoporous composite shows excellent stability in polar solvents.Results of catalytic tests indicate that the composite is an effective catalyst for oxidation of dibenzothiophen,and there are few activity losses even after the third cycle of uses.The high catalytic activity and good insolubility make it a promising catalyst in oxidative desulfurization process.
文摘Mesoporous SiO2-ZrO7 nanocomposite was successfully prepared by using supramolecular tfiblock copolymer as the template through evaporation-induced self-assembly approach. The textural and structural properties were characterized by X-ray diffraction, nitrogen adsorption analysis, and transmission electron microscope. Comparison between pure mesoporous silica and mesoporous silica-zirconia nanocomposite was also presented in this work. The surface area, pore size, and pore volume decreased as the Zr doping in the mesoporous silica framework. But the obtained nanocomposite maintained the cubic Im3m-type mesoporous structure.
基金Supported by the Natural Science Foundation of Heilongjiang Province(No.9810B).
文摘A mesoporous Al-Mg composite oxide with a hexagonal structure was synthesized with aluminium nitrate and magnesium nitrate as the reagents and sodium dodecyl sulfate（SDS） as the template in the presence of ethylenediamine. The XRD, nitrogen adsorption-desorption and TEM studies indicate that the composite has a hexagonal framework structure and an average pore diameter of 2. 6 nm. The TG/DTA spectra indicate that the decomposition and the removal of the occluded surfactant of the sample take place in a range of 230-550 ℃. The mesoporous Al-Mg composite oxide exhibites a highly catalytic activity for the oxyethylation of fatty alcohols. Narrow-range distributed ethoxylates are formed in the presence of the mesoporous Al-Mg composite oxide catalyst. The distribution selectivity coefficient（Cx） is 24 when the mesoporous Al-Mg composite oxide was used as a catalyst for the oxyethylation of octanol and the average adduct degree of ethoxylates is 6. 4.
基金Supported by the National Natural Science Foundation of China(2110311921407111 and 21277094)+7 种基金the Natural Science Foundation of Jiangsu Province(11KJB430012BK2012167 and BK20140280)the Scientific Research Foundation of the Chinese Ministry of Education([2013]693)the Excellent Innovation Team in Science and Technology of University in Jiangsuthe Province Collegiate Natural Science Fund of Jiangsu(14KJA43000412KJA430005)the Open Projects of the Jiangsu Key Laboratory for Environment Functional Materials(Nos.SJHG1310 and SJHG1304)the Science,Education and Health Foundation of Soochow(KJXW2013017)
文摘A novel mesoporous silica coated carbon composite(denoted SEG) with hierarchical pore structure has been successfully prepared in an aqueous solution that contains triblock copolymer template, aluminum chloride, siliceous source and expanded graphite. Textural property and morphology of the SEG composite were characterized by the combination of X-ray diffraction, N_2 adsorption–desorption, scanning electron microscopy,transmission electron microscopy and Fourier transform infrared measurements. Results show that mesoporous silica is steadily and uniformly grown on the surface of the graphite slices and the thickness of the silica layer can be finely tuned according to the silica/C molar ratio in the initial reaction solution. This newly synthesized SEG composite shows greatly increased adsorption capacity to methylene blue than the pristine expanded graphite in the batch tests. Both Langmuir and Frendlich models were further used to evaluate the adsorption isotherms of methylene blue over expanded graphite and SEG samples with different silica contents. Finally, pseudosecond-order model was used to describe the kinetics of methylene blue over expanded graphite and the silica-carbon composites.
基金supported by National Basic Research Program of China(2010CB732300,2013CB933201)National High Technology Research and Development Program of China(2011AA03A406,2012AA062703)+2 种基金the National Natural Science Foundation of China(21103048,21273150)Shu Guang Project of Shanghai Municipal Education CommissionShanghai Education Development Foundation(10SG30)
文摘Mesoporous CeO2-MnOx binary oxides with different Mn/Ce molar ratios were prepared by hydrothermal synthesis and characterized by scanning electron microscopy （SEM）, N2 sorption, X-ray diffraction （XRD）, X-ray photoelectron spectroscopy （XPS） and H2 temperature-programmed reduction （H2-TPR）. The characterization results indicated that the CeO2-MnOx catalysts exhibited flower-like microspheres with high specific surface areas, and partial Mn cations could be incorporated into CeO2 lattice to form solid solution. The CeO2-MnOx catalysts showed better catalytic activity for CO oxidation than that prepared by the coprecipitation method. Furthermore, the CeO2-MnOx catalyst with Mn/Ce molar ratio of 1 in the synthesis gel （Ce-Mn-1） exhibited the best catalytic activity, over which the conversion of CO could achieve 90% at 135 ℃. This was ascribed to presence of more Mn species with higher oxida- tion state on the surface and the better reducibility over the Ce-Mn-I catalyst than other CeO2-MnOx catalysts.
基金supported by Beijing Natural Science Foundation (No. 207001)the Funding Project for Academic Human Resources Development in Institutions of Higher Learning under the Jurisdiction of Beijing Munici-pality, and the Major State Basic Research Development Program of China (No. 2002CB211807)+1 种基金supported partly by the National Out-standing Youth Fund of China (No. 10125523 to Z.W.)the Knowledge Innovation Program of Chinese Academy of Sciences (KJCX2-SW-N11, KJCX2-SW -H12-02)
文摘A mesoporous LiFe0.99Mo0.01PO4/C composite was synthesized by the sol-gel method using （NH4）2MoO4 as a doping starting material. The formation of conductive carbon, metal doping and mesopores was achieved simultaneously in the prepared material. The characterizations of crystal structures and microstructures were investigated using X-ray diffraction （XRD）, scanning electron microscopy （SEM）, transmission electron microscopy （TEM）, extended X-ray-absorption fine-structure （EXAFS） and X-ray-absorption near-structure spectroscopy （XANES） while the surface area was determined using N2 adsorption techniques. Cyclic voltammetry （CV） and charge-discharge cycling performance were used to characterize its electrochemical properties. The sample possessed uniformly distributed mesopores with an average pore size of 4 nm, and the specific surface area was about 69.368 m^2/g. The results show that the reversible capacity of mesoporous LiFe0.99Mo0.01PO4/C is about 160 mAh/g at 0.1C, 135 mAh/g at 1C and 90 mAh/g at 5C, respectively. The capacity fading is neglectable.
基金supported by the National Key Research and Development Program of China(Grant No.2016YFB0101312)the National Natural Science Foundation of China(Grant No.21975157).
文摘t In this paper,a facile strategy is proposed to controllably synthesize mesoporous Li_(4)Ti_(5)O_(12)/C nanocomposite embedded in graphene matrix as lithium-ion battery anode via the co-assembly of Li_(4)Ti_(5)O_(12)(LTO)precursor,GO,and phenolic resin.The obtained composites,which consists of a LTO core,a phenolic-resin-based carbon shell,and a porous frame constructed by rGO,can be denoted as LTO/C/rGO and presents a hierarchical structure.Owing to the advantages of the hierarchical structure,including a high surface area and a high electric conductivity,the mesoporous LTO/C/rGO composite exhibits a greatly improved rate capability as the anode material in contrast to the conventional LTO electrode.
