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生物质气经由二甲醚两步法制备低碳烯烃

ISSN号：1674-0068
期刊名称：《化学物理学报》
时间：0
分类：R-33[医药卫生]
作者机构：[1]中国科学院广州能源研究所可再生能源重点实验室,广州110640, [2]中国科学院大学,北京100049
相关基金：ACKNOWLEDGM ENTS This work was supported by the National Natural Science Foundation of China （No.51006110, No.51276183, and No.51036006）, the National Natural Research Foundation of China/Japan Science and Technology Agency （No.51161140331）, and National Key Basic Research Program 973 Project Founded by MOST of China （No.2013CB228105）.

作者：李宇萍[1], 涂军令[1,2], 王铁军[1], 马隆龙[1], 张兴华[1], 章青[1], 蔡炽柳[1]

关键词：低碳烯烃, 二甲醚, 两步转化, NiSAPO-34, HZSM-5, 生物质气, Light olefins, Two-stage conversion, Dimethyl ether, Biosyngas, NiSAPO-34/HZSM-5

中文摘要：

制备出NiSAPO-34及NiSAPO-34／HZSM-5催化剂，考察了其对二甲醚催化转化制备低碳烯烃的性能．利用Cu／Zn／Al／HZSM-55u筛选出的2％NiSAPO—34／HZSM-5催化剂进行生物质气经由二甲醚两步法制备低碳烯烃的实验，结果表明在SAPO-34上添2H2％的Ni不改变其结构，但降低了酸中心数量，并生成了较强的酸中心．添加少量具有稳定酸中心的HZSM-5，该催化剂的活性提高到3h以上，反应进行2h获得了最高的低碳烯烃选择性为90．8％．当把该催化剂应用到两步催化转化过程的第二个反应器中，其高催化活性可达5h以上．当以低氢碳比生物质气（H2／CO／CO2／N2／CH4=41．5／26．9／14．2／14．6／2．89）作为原料时，经两步转化，低碳烯烃的收率达到84．6g／m^3syngas.

英文摘要：

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.

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