One-pot N-alkylation of primary amines to secondary amines by gold clusters supported on porous coordination polymers

One-pot N-alkylation of primary amines to secondary amines by gold clusters supported on porous coordination polymers
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DOI:
10.1007/bf03214948
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发表时间:
2009-01-01
期刊:
影响因子:
2.2
通讯作者:
Haruta, Masatake
Haruta, Masatake
中科院分区:
工程技术4区
文献类型:
--
作者:
Ishida, Tamao;Kawakita, Noriko;Haruta, Masatake

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采用固相研磨法在三种多孔配位聚合物(PCF):MOF-5、CIPIL-2和Al-MIL 53上制备了金团簇和纳米粒子。Au粒子的尺寸取决于PCP的种类,并且按照Al-MIL 53 < CPL-2 < MOF-5的顺序增大。用HAADF-STEM法测得Al-MIL 53上负载的Au颗粒的平均直径为1.6 nm。这种小的Au团簇在Al-MIL 53上可以催化伯胺通过顺序氧化/氢化一锅法合成仲胺,这是由于亚胺的氢化效率显著提高。沉积在Al-MIL 53上的金簇也可以促进胺与醇在N-2气氛下的N-烷基化反应,形成仲胺,而不使用O-2和H-2。
Gold clusters and nanoparticles were deposited on the three kinds of porous coordination polymers (PCPs), MOF-5, CIPIL-2, and Al-MIL53 by the solid grinding method. The size of Au particles depended on the kinds of PCPs and increased in the order of Al-MIL53 < CPL-2 < MOF-5. The mean diameter of Au particles supported on Al-MIL53 was estimated to be 1.6 nm by HAADF-STEM. Such small Au clusters on Al-MIL53 can catalyze one-pot synthesis of secondary amines from primary amines by sequential oxidation/hydrogenation owing to the remarkable improvement of hydrogenation efficiency of imine. Gold clusters deposited on Al-MIL53 can also promote N-alkylation of amine with alcohol to form a secondary amine under N-2 atmosphere without using O-2 and H-2.