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碳纳米管促进的Co-Cu氧化物基低碳醇合成催化剂的制备研究

期刊名称：厦门大学学报 (自然科学版), 2007, 46(6): 792-799
时间：0
分类：O643.3[理学—物理化学;理学—化学]
作者机构：[1]厦门大学化学化工学院化学系,固体表面物理化学国家重点实验室,福建厦门361005
相关基金：国家重点基础研究发展规划（973）项目（2005CB221403）,国家自然科学基金项目（20473063和20590364）和福建省科技重大项目（2005HZ01-3）共同资助
相关项目：能源发展中的若干关键化学科学基础问题

关键词：碳纳米管促进剂, 低碳醇合成, Co-Cu氧化物基催化剂, multiwalled carbon nanotube promoter, higher alcohol synthesis, Co-Cu oxide-based catalyst

中文摘要：

用自行制备的多壁碳纳米管（MWCNTs）作为添加剂,制备一类用于合成气制低碳醇的共沉淀型MWCNTs掺合的Co-Cu催化剂（CoiCuj-x%MWCNTs）.催化剂组成的优化结果显示：MWCNTs的添加量及Co、Cu两种金属组分的相对含量（摩尔比）对低碳醇合成（HAS）反应活性和产物选择性的影响显著;MWCNTs的添加量以11%为佳,Co/Cu摩尔比以3∶1为宜.在所制备的Co3Cu1-11%MWCNTs催化剂上,5.0 MPa、573 K、V（H2）/V（CO）/V（CO2）/V（N2）=45/45/5/5和GHSV=10 000 mL/（h.g）的反应条件下,CO的转化率可达39.1%,总（C1~8）醇和二甲醚（DME）的C-基选择性合计达到74.3%,C2~8-醇和DME的时空产率合计达1 072 mg/（h.g）;在含氧产物中,S（C2~8-醇＋DME）/S（MeOH）=17.8（C-基选择性比）,展现其作为燃料油品添加剂的应用前景.催化剂的制备表征研究揭示,氧化态前驱物中高度分散的CuCo2O4尖晶石微晶相的形成对于营造/产生低碳醇合成所需固溶体型双金属CoiCuj催化活性位至关重要;MWCNTs促进的催化剂对氢吸附、活化的优异性能在促进催化剂活性和选择性的提高、以及抑制水煤气变换副反应等方面都可能起重要作用.

英文摘要：

Using the homemade multi-walled carbon nanotubes（MWCNTs）as additive,a type of MWCNT-doped Co-Cu oxide catalyst（noted as CoiCuj-x% MWCNTs）for higher alcohol synthesis（HAS）was prepared by co-precipitation method. It was experimentally shown that MWCNT-adding amount and Co/Cu molar ratio have marked effect on the reactivity and selectivity of HAS,and that the optimal MWCNT-adding amount was 11% （mass percentage）and the optimal Co/Cu molar ratio was 3 ： 1. Over a Co3Cu,-11% MWCNTs catalyst under reaction conditions of 5.0 MPa,573 K,V（H2 ）/V（CO）/V（CO2）/V（N2 ）=45/45/5/5,GHSV=10000 mL/ （h · g）, the observed CO-conversion reached 39.1%, and the selectivity of total（C1-8）alcohols and dimethyl ether（DME）combined reached 74. 3%,and the corresponding space-time-yield（STY）of C2-8 alcohols and DME combined reached 1072 mg/（h · g）, the S （C2-8-alc. ＋ DME）/S（MeOH） = 17.8 （C-based selectivity ratio） in the obtained total oxygenated products, a good prospect for such oxygenated products to be used as gasoline additives. The results of catalyst characterizations revealed that in the process of catalyst preparation,the formation of highly dispersed CuCo2O4 spinel crystallite phase in the oxide precursor of catalyst was utmost important for generation,through He-reduction,of solid-solution-type bimetal Co;Cuj sites catalytically active for HAS. The excellent performate of the MWCNT-promoted catalyst for adsorption and activation of H2 played important role in enhancing the reactivity and selectivity of HAS and inhibiting the side-reaction of water-gas-shift（WGS）.