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国家自然科学基金(51276183)

作品数:4 被引量:11H指数:2
相关作者:马隆龙王铁军李宇萍定明月张琦更多>>
相关机构:中国科学院中国科学院大学更多>>
发文基金:国家自然科学基金国家重点基础研究发展计划更多>>
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乙二醇促进制备高分散的Co/SiO_2催化剂及其催化乳酸乙酯转化为1,2-丙二醇的气相加氢活性(英文)被引量:1
2016年
研究了利用乙二醇共浸渍方法制备高分散的二氧化硅负载钴催化剂,该催化剂有效地提高了乳酸乙酯的气相加氢反应活性。系统地考察了钴金属负载量、乙二醇与硝酸钴摩尔比、醇种类和焙烧温度等制备参数对四氧化三钴纳米粒子物性的影响。乙二醇与硝酸钴摩尔比和醇种类对二氧化硅负载的四氧化三钴纳米粒子大小有显著影响。与常规的浸渍方法相比较,共浸渍过程中的乙二醇增强了二价钴粒子和载体二氧化硅之间的相互作用力,从而引起金属钴分散度的提高以及四氧化三钴纳米粒子粒径从16 nm降到5 nm以下;金属钴的高分散与无定型硅酸钴的形成密切相关;同时显著地提高了乳酸乙酯的加氢活性,在反应条件下(2.5MPa、160°C和10%(w,质量分数)Co/SiO_2)乳酸乙酯的转化率从69.5%提高到98.6%,1,2-丙二醇的选择性达到98.0%。利用X射线衍射(XRD)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)、N_2吸脱附实验、H_2程序升温还原(H_2-TPR)等表征手段对共浸渍制备的Co/SiO_2催化剂结构和形貌进行了表征分析。
仇松柏翁育靖刘琪英马隆龙张琦王铁军
关键词:1,2-丙二醇乙二醇
Effect of Calcination Temperature on Catalytic Activity and Textual Property of Cu/HMOR Catalysts in Dimethyl Ether Carbonylation Reaction被引量:3
2013年
The effect of calcination temperature on the catalytic activity for the dimethyl ether (DME) carbonylation into methyl acetate (MA) was investigated over mordenite supported copper (Cu/HMOR) prepared by ion-exchange process. The results showed that the catalytic activity was obviously affected by the calcination temperature. The maximal DME conversion of 97.2% and the MA selectivity of 97.9% were obtained over the Cu/HMOR calcined at 430 ℃ under conditions of 210 ℃, 1.5 MPa, and GSHV of 4883 h^-1. The obtained Cu/HMOR catalysts were characterized by powder X-ray diffraction, N2 absorption, NH3 temperature program desorption, CO temperature program desorption, and Raman techniques. Proper calcination temperature was effective to promote copper ions migration and diffusion, and led the support HMOR to possess more acid activity sites, which exhibited the complete decomposing of copper nitrate, large surface area and optimum micropore structure, more amount of CO adsorption site and proper amount of weak acid centers.
张雪李宇萍仇松柏王铁军马隆龙张琦定明月
关键词:CARBONYLATION
Production of Light Olefins from Biosyngas by Two-stage Catalytic Conversion Process via Dimethyl Ether被引量:1
2014年
NiSAPO-34 and NiSAPO-34/HZSM-5 were prepared and evaluated for the performance of dimethyl ether (DME) conversion to light olefins (DTO). The processes of two-stage light olefin production, DME synthesis and the following DTO, were also investigated using biosyngas as feed gas over Cu/Zn/A1/HZSM-5 and the optimized 2%NiSAPO-34/HZSM- 5. The results indicated that adding 2%Ni to SAPO-34 did not change its topology structure, but resulted in the forming of the moderately strong acidity with decreasing acid amounts, which slightly enhanced DME conversion activity and C2=-C3= selectiw ity. Mechanically mixing 2%NiSAPO-34 with HZSM-5 at the weight ratio of 3.0 further prolonged DME conversion activity to be more than 3 h, which was due to the stable acid sites from HZSM-5. The highest selectivity to light olefins of 90.8% was achieved at 2 h time on stream. The application of the optimized 2%NiSAPO-34/HZSM-5 in the second-stage reactor for DTO reaction showed that the catalytic activity was steady for more than 5 h and light olefin yield was as high as 84.6 g/m3syngas when the biosyngas (H2/CO/CO2/N2/CH4=41.5/26.9/14.2/14.6/2.89, vol%) with low H/C ratio of 1.0 was used as feed gas.
李宇萍涂军令王铁军马隆龙张兴华章青蔡炽柳
Hβ改性Co/SiO2对费托合成航空燃油类烃的影响被引量:6
2014年
在中孔SiO2(SG)和微孔Hβ分子筛(Si/Al=25、60、80)组成的复合载体上,制备了多功能Co基费托合成催化剂,考察了其合成航空燃油类烃(C8-C18)的性能。XRD、FTIR、H2-TPR、N2-物理吸附研究表明:Hβ的引入,使得Co/SG/Hβ催化剂具有一定酸性和微孔结构。随分子筛硅铝比的降低,催化剂红外图谱的特征波数向低波数移动,酸性有所提高,中孔 SiO2消弱了其酸性及载体与金属粒子相互作用,提高了 Co分散和还原度及加氢活性。Hβ的微孔结构和酸性促进了初级产物裂解及异构化反应,提高了异构烃类选择性。Co/SG/Hβ(80)催化剂较大的比表面积和微孔体积及适当的酸性中心是其高活性(CO转化率95.7%)及高航空燃油类烃选择性(42.3%,其中异构烃为27.6%)的关键因素。
李宇萍王铁军马隆龙吴创之定明月
关键词:COSIO2催化剂HΒ分子筛费托合成孔结构
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