An immature pinecone shaped hierarchically structured zirconia (ZrO2-ipch) and a cobblestone-like zirconia nanoparticulate (ZrO2-cs), both with the monoclinic phase (m-phase), were synthesized by the facile hydr...An immature pinecone shaped hierarchically structured zirconia (ZrO2-ipch) and a cobblestone-like zirconia nanoparticulate (ZrO2-cs), both with the monoclinic phase (m-phase), were synthesized by the facile hydrothermal method and used as the support for a Ni catalyst for the dry reforming of methane (DRM) with CO2. ZrO2-ipch is a much better support than ZrO2-cs and the traditional ZrO2 irregular particles made by a simple precipitation method (ZrO2-ip). The supported Ni catalyst on ZrO2-ipch (Ni/ZrO2-ipch) exhibited outstanding catalytic activity and coke-resistant stability compared to the ones on ZrO2-cs (Ni/ZrO2-cs) and ZrO2-ip (Ni/ZrO2-ip). Ni/ZrO2-ip exhibited the worst catalytic performance. The origin of the significantly enhanced catalytic performance was revealed by characterization including XRD, N2 adsorption measurement (BET), TEM, H2-TPR, CO chemisorption, CO2-TPD, XPS and TGA. The superior catalytic activity of Ni/ZrO2-ipch to Ni/ZrO2-cs or Ni/ZrO2-ip was ascribed to a higher Ni dispersion, increased reducibility, enhanced oxygen mo- bility, and more basic sites with a higher strength, which were due to the unique hierarchically structural morphology of the ZrO2-ipch support. Ni/ZrO2-ipch exhibited better stability for the DRM reaction than Ni/ZrO2-ip, which was ascribed to its higher resistance to Ni sintering due to a strengthened metal-support interaction and the confinement effect of the mesopores and coke deposition resistance. The higher coking resistance of Ni/ZrO2-ipch for the DRM reaction in comparison with Ni/ZrOz-ip orignated from the coke-removalabitity of the higher amount of lattice oxygen and more basic sites, confirmed by XPS and CO2-TPD analysis, and the stabilized Ni on the Ni/ZrO2-ipch catalyst by the confinement effect of the mesopores of the hierarchical ZrO2-ipch sup- port. The superior catalytic performance and coking resistance of the Ni/ZrO2-ipch catalyst makes it a promising candidate for synthesis gas production from the DRM reaction.展开更多
The synthesis procedures and physical properties of the ambient dried hydrophobic silica aerogels by using different contents of ethanol (EtOH)/trimethylchlorosilane (TMCS)/n-Hexane as surface modification agent w...The synthesis procedures and physical properties of the ambient dried hydrophobic silica aerogels by using different contents of ethanol (EtOH)/trimethylchlorosilane (TMCS)/n-Hexane as surface modification agent were investigated. One-step solvent exchange and surface modification were simultaneously progressed by immersing silica hydrogels in EtOH/TMCS/n-Hexane solution. It is found that microstructures as well as properties of silica aerogels like porosity, specific density and specific surface area are affected by the contents of surface modification agent in the sol from the results of SEM, TEM morphology, FT-IR chemical structure, BET surface area and BJH pore size analyses. The volume of TMCS is of 10% and 20% of hydrogels, and the final product is hydrophilic xerogels. When TMCS's percent (v/v) is elevated to 75 %-100%, hydrophobic silica aerogels with good performance are synthesized, the porosities of aerogels are in the range of 93.5%-95.8% and the average pore size diameter is less than 20 nm.展开更多
SAPO-34 is one of the main catalysts used in the petrochemical industry. Various effective methods have been developed to synthesize SAPO-34 with optimal size and characteristics for such application, In the present s...SAPO-34 is one of the main catalysts used in the petrochemical industry. Various effective methods have been developed to synthesize SAPO-34 with optimal size and characteristics for such application, In the present study, SAPO-34 was synthesized using a dry gel method at high temperatures. Morpholine was used as an organic template. The products were characterized by X-ray diffraction, field-emission scan- ning electron microscopy, energy-dispersive X-ray spectroscopy, and gas sorption analysis, The results showed that application of the dry gel method at high temperatures successfully afforded a pure catalyst with high crystallinity, Small particles of less than 500 nm could be obtained within a short reaction time of 30 min.展开更多
基金financially supported by the Joint Fund of Coal, set up by National Natural Science Foundation of China and Shenhua Co., Ltd.(U1261104)the National Natural Science Foundation of China (21276041)+3 种基金the Program for New Century Excellent Talents in University (NCET-12-0079)the Natural Science Foundation of Liaoning Province (2015020200)the Fundamental Research Funds for the Central Universities (DUT15LK41)the Science and Technology Development Program of Hangzhou (20130533B14)~~
文摘An immature pinecone shaped hierarchically structured zirconia (ZrO2-ipch) and a cobblestone-like zirconia nanoparticulate (ZrO2-cs), both with the monoclinic phase (m-phase), were synthesized by the facile hydrothermal method and used as the support for a Ni catalyst for the dry reforming of methane (DRM) with CO2. ZrO2-ipch is a much better support than ZrO2-cs and the traditional ZrO2 irregular particles made by a simple precipitation method (ZrO2-ip). The supported Ni catalyst on ZrO2-ipch (Ni/ZrO2-ipch) exhibited outstanding catalytic activity and coke-resistant stability compared to the ones on ZrO2-cs (Ni/ZrO2-cs) and ZrO2-ip (Ni/ZrO2-ip). Ni/ZrO2-ip exhibited the worst catalytic performance. The origin of the significantly enhanced catalytic performance was revealed by characterization including XRD, N2 adsorption measurement (BET), TEM, H2-TPR, CO chemisorption, CO2-TPD, XPS and TGA. The superior catalytic activity of Ni/ZrO2-ipch to Ni/ZrO2-cs or Ni/ZrO2-ip was ascribed to a higher Ni dispersion, increased reducibility, enhanced oxygen mo- bility, and more basic sites with a higher strength, which were due to the unique hierarchically structural morphology of the ZrO2-ipch support. Ni/ZrO2-ipch exhibited better stability for the DRM reaction than Ni/ZrO2-ip, which was ascribed to its higher resistance to Ni sintering due to a strengthened metal-support interaction and the confinement effect of the mesopores and coke deposition resistance. The higher coking resistance of Ni/ZrO2-ipch for the DRM reaction in comparison with Ni/ZrOz-ip orignated from the coke-removalabitity of the higher amount of lattice oxygen and more basic sites, confirmed by XPS and CO2-TPD analysis, and the stabilized Ni on the Ni/ZrO2-ipch catalyst by the confinement effect of the mesopores of the hierarchical ZrO2-ipch sup- port. The superior catalytic performance and coking resistance of the Ni/ZrO2-ipch catalyst makes it a promising candidate for synthesis gas production from the DRM reaction.
基金Funded by the National Mega-Project of Scientific & Technical Sup-porting Programs, Ministry of Science & Technology of China(No.2006BAJ04A 04)the Science Foundation of Liaoning Province,China (No.20062147)
文摘The synthesis procedures and physical properties of the ambient dried hydrophobic silica aerogels by using different contents of ethanol (EtOH)/trimethylchlorosilane (TMCS)/n-Hexane as surface modification agent were investigated. One-step solvent exchange and surface modification were simultaneously progressed by immersing silica hydrogels in EtOH/TMCS/n-Hexane solution. It is found that microstructures as well as properties of silica aerogels like porosity, specific density and specific surface area are affected by the contents of surface modification agent in the sol from the results of SEM, TEM morphology, FT-IR chemical structure, BET surface area and BJH pore size analyses. The volume of TMCS is of 10% and 20% of hydrogels, and the final product is hydrophilic xerogels. When TMCS's percent (v/v) is elevated to 75 %-100%, hydrophobic silica aerogels with good performance are synthesized, the porosities of aerogels are in the range of 93.5%-95.8% and the average pore size diameter is less than 20 nm.
文摘SAPO-34 is one of the main catalysts used in the petrochemical industry. Various effective methods have been developed to synthesize SAPO-34 with optimal size and characteristics for such application, In the present study, SAPO-34 was synthesized using a dry gel method at high temperatures. Morpholine was used as an organic template. The products were characterized by X-ray diffraction, field-emission scan- ning electron microscopy, energy-dispersive X-ray spectroscopy, and gas sorption analysis, The results showed that application of the dry gel method at high temperatures successfully afforded a pure catalyst with high crystallinity, Small particles of less than 500 nm could be obtained within a short reaction time of 30 min.