有机化学 ›› 2020, Vol. 40 ›› Issue (1): 226-231.DOI: 10.6023/cjoc201906022 上一篇    下一篇

研究简报

新型膦胺配体羰基钌化合物的合成及其催化性能研究

方霄龙a,b, 章敏a, 段宁a, 汪新a, 朱红平b   

  1. a 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;
    b 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
  • 收稿日期:2019-06-18 修回日期:2019-08-22 发布日期:2019-09-12
  • 通讯作者: 汪新, 朱红平 E-mail:wangxin164@sina.com;hpzhu@xmu.edu.cn
  • 基金资助:
    国家自然科学基金(Nos.21802010,21673191)、安徽省自然科学基金(No.1808085QB48)及池州学院青年教师科研启动基金(No.2018YJRC001)资助项目.

Synthesis and Catalytic Property of New Aminophosphino Ruthenium Carbonyl Complexes

Fang Xiaolonga,b, Zhang Mina, Duan Ninga, Wang Xina, Zhu Hongpingb   

  1. a Key Laboratory of Micro-nano Powder and Advanced Energy Materials of Anhui Higher Education Institutes, College of Chemistry and Materials Engineering, Chizhou University, Chizhou, Anhui 247000;
    b 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
  • Received:2019-06-18 Revised:2019-08-22 Published:2019-09-12
  • Supported by:
    Project supported by the National Natural Science Foundation of China (Nos. 21802010, 21673191), the Natural Science Foundation of Anhui Province (No. 1808085QB48) and the Starting Grants for Young Teachers of Chizhou University (No. 2018YJRC001).

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)Ru3μ-H)(CO)92)、(o-PPh2C6H4NH)2Ru(CO)23)和(μ-o-PPh2C6H4NMe22Ru(CO)34).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24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.

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

New carbonyl ruthenium complexes (μ-o-PPh2C6H4NH)Ru3(μ-H)(CO)9 (2), (o-PPh2C6H4NH)2Ru(CO)2 (3) and (μ-o-PPh2C6H4NMe2)2Ru(CO)3 (4) have been successfully synthesized by using ruthenium carbonyl and o-PPh2C6H4NR2 (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.

Key words: aminophosphino ruthenium carbonyl, synthesis and characterization, catalytic hydrogenation, structure and property, deactivation