新型膦胺配体羰基钌化合物的合成及其催化性能研究  

Synthesis and Catalytic Property of New Aminophosphino Ruthenium Carbonyl Complexes

作　　者：方霄龙 章敏 段宁 汪新[1] 朱红平[2] Fang Xiaolong;Zhang Min;Duan Ning;Wang Xin;Zhu Hongping(Key Laboratory of Micro-nano Powder and Advanced Energy Materials ofAnhui Higher Education Institutes,College of Chemistry and Materials Engineering,Chizhou University,Chizhou,Anhui 247000;State Key Laboratory of Physical Chemistry of Solid Surfaces,National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen,Fujian 361005)

机构地区：[1]池州学院化学与材料工程学院,微纳粉体与先进能源材料安徽普通高校重点实验室,安徽池州247000 [2]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,醇醚酯清洁生产国家工程实验室,福建厦门361005

出　　处：《有机化学》2020年第1期226-231,共6页Chinese Journal of Organic Chemistry

基　　金：国家自然科学基金(Nos.21802010,21673191);安徽省自然科学基金(No.1808085QB48);池州学院青年教师科研启动基金(No.2018YJRC001)资助项目。

摘　　要：以十二羰基三钌和o-PPh2C6H4NR2(R=H,Me)配体为原料,成功制备了三种新型羰基钌化合物(μ-o-PPh2-C6H4NH)Ru3(μ-H)(CO)9(2)、(o-PPh2C6H4NH)2Ru(CO)2(3)和(μ-o-PPh2C6H4NMe2)2Ru(CO)3(4).对这三个化合物进行了核磁共振和红外谱学、元素分析和X射线单晶衍射分析表征,并对这三个化合物进行了催化性能研究.化合物2和4可催化苯甲醛加氢反应生成苯甲醇,但是3没有催化活性.从实验角度阐述了膦胺配体钌催化剂的结构与性能关联,进一步探讨了加氢催化反应失活的可能原因.New carbonyl ruthenium complexes(μ-o-PPh2 C6 H4 NH)Ru3(μ-H)(CO)9(2),(o-PPh2 C6 H4 NH)2 Ru(CO)2(3) and(μ-o-PPh2 C6 H4 NMe2)2 Ru(CO)3(4) have been successfully synthesized by using ruthenium carbonyl and o-PPh2 C6 H4 NR2(R=H, Me) ligand. The three complexes have all been characterized by NMR and IR spectroscopies, elemental analysis and X-ray crystallography. Complexes 2 and 4 could catalyze the hydrogenation of benzaldehyde into benzyl alcohol. However, complex 3 showed no activity. This study reveals a correlation between structure and catalytic property, where the possible deactivation mode for the hydrogenation reaction using the aminophosphino ruthenium catalyst is discussed in view of the experimental work.

关 键 词：膦胺配体羰基钌化合物 合成与表征 催化加氢 结构与性能 失活 

分 类 号：O643.36[理学—物理化学] O641.4[理学—化学]