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新型膦胺配体羰基钌化合物的合成及其催化性能研究

本站小编 Free考研考试/2022-02-14

摘要/Abstract



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


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