MOF衍生Rh/ZrO_2@C催化剂的制备及氢甲酰化性能研究

MOF derived Rh/ZrO_2@C catalyst for hydroformylation of alkenes

以UIO-66为前驱体,通过高温惰性气氛下焙烧得到ZrO_2@C载体,采用吸附还原方法制备了1%Rh/ZrO_2@C催化剂。通过X射线衍射、热重、高分辨透射电镜等对催化剂结构进行分析,结果表明,金属Rh在载体上高度分散。将所合成的催化剂用于1-十二烯的氢甲酰化反应,考察了反应温度和反应压力对催化剂性能的影响。结果表明,当反应温度为90℃、反应压力为4 MPa时,催化剂具有较好的催化性能,1-十二烯转化率为94. 2%,十三醛选择性达到98. 9%,且催化剂循环使用4次后,活性无明显下降。

ZrO2@C carrier is obtained by calcining UIO-66 materials under inert atmosphere at high temperature.The 1%Rh/ZrO2@C catalyst is prepared through adsorption reduction method.XRD,TG and HRTEM measurements are used to characterize the obtained catalysts.The results indicate that metal Rh disperses highly on the carrier.Hydroformylation reaction of 1-dodecene is applied to evaluate the catalytic performance of 1%Rh/ZrO2@C catalyst.Influences of reaction temperature and pressure on the performance of catalyst are investigated.It is shown that the catalyst exhibits good catalytic performance at 90℃and 4 MPa,the conversion of 1-dodecene can achieve about 94.2%and the selectivity of tridecylic aldehyde reaches 98.9%.Moreover,there is no obvious loss in catalytic activity after the catalyst has been reused 4 times.