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机构地区:[1]中国科学院大连化学物理研究所 [2]中国科学院研究生院,北京100049
出 处:《催化学报》2005年第9期824-828,共5页
基 金:国家自然科学基金(20176057;20490200);国际科技合作重点项目计划(2001CB711203);中国科学院大连化学物理研究所创新基金(K2003E2)资助项目.
摘 要:研究了Ru/ZrO2蜂窝陶瓷整体催化剂对苯液相选择加氢制环己烯反应的催化性能,考察了催化剂载体、活性组分含量、预处理条件、反应温度、反应压力、水和硫酸锌水溶液等对该反应的影响. 结果表明,整体催化剂不经预还原就可以直接进行苯液相加氢反应; 反应物中不加水或其它无机添加剂时环己烯的选择性为0,水或硫酸锌水溶液的加入大大降低了反应活性,但环己烯的选择性显著提高,约达到20%; 反应物中水和苯有最优配比,以保证最佳的环己烯选择性和收率; 反应温度在413~443 K,反应压力为3~4 MPa,硫酸锌浓度为0.1 mol/L时,反应结果较好.An attractive field of industrial use of a monolithic reactor lies in multiphase catalytic reactions, especially hydrogenation and oxidation of hydrocarbons, due to its superior interphase mass transfer performance. In this paper, liquid-phase selective hydrogenation of benzene to cyclohexene over a Ru/ZrO2 honeycomb monolithic catalyst was studied in detail. The effects of catalyst and reaction variables, such as the support type, ruthenium content, catalyst pretreatment, addition of water or salt in reactants, reaction temperature, hydrogen pressure and volume ratio of water to benzene, on the performance of the reaction were investigated. Good yields of cyclohexene could be obtained using ruthenium particles supported on hydrophilic oxides, like silica, alumina, titania and zirconia. It should be noted that the reaction can occur without catalyst prereduction in hydrogen flow in the monolithic reactor. No cyclohexene was detected in the absence of reaction additives such as water or ZnSO4 solution, but the selectivity for cyclohexene dramatically increased to higher than 20 % when these reaction modifiers were added. There existed an optimum volume ratio of water to benzene for high yield of cyclohexene. Better results were achieved in the presence of 0.1 mol/L ZnSO4 under the reaction temperatures of 413- 443 K and pressures of 3- 4 MPa.
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