介孔分子筛MCM-41负载钌配合物的合成及其对醇氧化反应的催化性能

Synthesis and efficient catalysis for alcohol oxidaton of mesoporous molecular sieves MCM-41 immobilized ruthenium complex

通过多步接枝法将钌配合物Ru(Terpyridine)(PPh_3)Cl_2(Ru(Terpy)(PPh_3)Cl_2)负载到MCM-41分子筛上,得到固载化的MCM-41/Ru(Terpy)(PPh_3)Cl_2催化剂.采用FT-IR、UV-Vis、XRD、ICP、N2吸附等手段对催化剂及其中间体进行了表征.将其与TBHP组成催化氧化体系,用于仲醇的选择性氧化反应.考察了该催化氧化体系的催化性能,结果表明,在80℃无溶剂条件下可高活性地催化仲醇氧化生成相应的酮.实验结果还表明该催化剂的循环使用性能较差.红外光谱分析表明其之所以失活是因为在反应过程中发生有机配体三苯基膦的脱落.

The ruthenium complex Ru（Terpy）（PPh_3）Cl_2 was successfully grafted onto MCM-41 by a multi-step grafting method to obtain the immobilized MCM-41/Ru（Terpy）（PPh_3）Cl_2 catalyst. The immobilized ruthenium complex and the intermediates were characterized by FT-IR, UV-Vis, XRD, ICP analysis and N2 adsorption. The catalytic system was used for the oxidation of secondary alcohols with TBHP as terminal oxidant. The results showed that the secondary alcohols could be efficiently oxidized to the corresponding ketones at 80 ℃ without presence of solvent. Unfortunately, the catalyst showed poor reusability and its activity decreased quickly due to the leaking of the triphenylphosphine ligand during the catalytic run.