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碳纳米管负载合成气制低碳醇Co-Mo-K硫化物基催化剂

期刊名称：厦门大学学报(自然科学版), 2006, 45(6): 797-804
时间：0
分类：O643[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,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973项目（2005CB221400）和国家自然科学基金项目（20473063,20590364）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：多壁碳纳米管, 碳纳米管负载CoMoK硫化物基催化剂, 低碳醇合成, 合成气催化转化, Multi-walled carbon nanotubes, CNT-supported CoMoK-sulfide catalyst, higher alcohol synthesis, syngas catalytic conversion

中文摘要：

用自行制备的多壁碳纳米管（CNTs）作为载体，制备一类负载型CNTs促进Co—Mo—K硫化物基催化剂，x％CoiMojKk／CNTs（x％为质量百分数）．实验发现，在2．0MPa、593K、y（CO）：V（H2）：V（N2）=45：45：10、GHSV=2400mLSTP·h^-1·g-caL^-1的反应条件下，在11．6％Co1Mo1K0.6／CNTs催化剂上，所观测低碳醇合成的比反应速率达到0．77μmol-CO·s^-1·（mmol—Mo）^-1．是AC和γ-Al2O3分别负载各自最佳Co-Mo-K摩尔组成及相应负载量催化剂（50．3％Co1Mo1K0.5／AC和26．1％Co1Mo1K0.8／γ-Al2O3）上这个值（分别为0．23和0．27μmol-CO·s^-1·（mmol-Mo）^-1）的3．35和2．85倍．对比研究显示，用CNTs代替常规载体AC和γ-Al2O3并不引起所负载Co1Mo1K0.6硫化物催化剂上低碳醇合成反应的表观活化能发生明显变化．与AC或γ-Al2O3负载的参比体系相比，CNTs负载的催化剂更易于在较低温度下还原活化．并促使工作态催化剂表面催化活性Mo物种（Mo^1＋）在总Mo量中所占份额明显提高；在另一方面，CNTs负载的催化剂展现出对H2更强的吸附活化能力，有助于在工作态催化剂表面营造较高稳态浓度吸附氢的表面氛围，于是提高了表面加氢反应的速率；这些因素对低碳醇合成反应活性的提高都有重要贡献．

英文摘要：

With home-made multi-walled carbon nanotubes（MWCNTs,simplified as CNTs）as support, CNT-supported Co-Mo-K sulfide catalysts,denoted as x% （mass percentage） CoiMojKk/CNTs, were prepared. Their catalytic performance for higher alcohol synthesis（HAS）from syngas was evaluated,and compared with the reference system supported by AC or γ-Al2O3. Over the 11.6% Co1Mo1K0.6/CNTs catalyst under reaction condition of 2.0 MPa,593 K,V（CO）： V（H2）： V（N3）=45 ： 45 ： 10 and GHSV=2 400 mLSTP·h^-1 · gcsL^-1 ,the specific reaction rate of HAS reached 0.77 μmol-CO · s^-1 · （mmol-Mo）^-1 ,which was 3.35 and 2.85 times as high as that [0.23 and 0.27 μmol-CO · s^-1 · （mmol-Mo）^-1] of the reference systems supported by AC and γ-Al2O3 with the respective optimal molar composition and loading amount of CoiMojKk, S0. 3 % Co1Mo1K0.8 / AC and 26. 1% Co1Mo1K0.8/γ-Al2O3 ,respectively. It was experimentally found that using the CNTs in place of AC or γ-Al2O3 as support of the catalyst caused little change in the apparent activation energy for the HAS reaction, but led to a significant increase in concentration of catalytically active Mo-species（Mo^4＋）at the surface of the functioning catalyst. On the other hand, H2-TPD measurements revealed that the CNT- supported catalyst could reversibly adsorb a greater amount of hydrogen under atmospheric pressure at temperatures ranging from room temperature to ～673 K. This unique feature would help to generate microenvironments with higher stationary-state concentration of active hydrogen-adspecies at the surface of the functioning catalyst. Both factors mentioned above were favorable to increasing the rate of HAS reactions.