Rh(OH)_x/TS-1@KCC-1双功能催化剂上一锅反应合成伯酰胺(英文)  

One-pot synthesis of primary amides on bifunctional Rh(OH)_x /TS-1@KCC-1 catalysts

作　　者：彭洪根[1] 王达锐[1] 徐乐[1] 吴鹏[1] 

机构地区：[1]华东师范大学化学系上海市绿色化学与化工过程绿色化重点实验室,上海200062

出　　处：《催化学报》2013年第11期2057-2065,共9页

基　　金：supported by the National Natural Science Foundation of China (220925310, U1162102);the Specialized Research Fund for the Doc-toral of Higher Education (2012007613000);the National Basic Research Program of China (973 Program, 2012BAE05B02);the Shanghai Lead-ing Academic Discipline Project (B409)~~

摘　　要：在微乳液体系中成功地将花瓣状介孔氧化硅微球(KCC-1)包覆在钛硅分子筛TS-1表面,得到了一种新型微孔/介孔复合核壳结构材料TS-1@KCC-1.详细考察了TS-1@KCC-1的合成条件及可能的形成机理.适宜的合成温度及时间分别为373–393 K和4h.壳层厚度可方便地通过改变硅源正硅酸乙酯和TS-1的比例在25–80 nm间进行调控.以TS-1@KCC-1为载体负载Rh(OH)x后即得到双功能催化材料Rh(OH)x/TS-1@KCC-1,该材料同时具有Ti和Rh(OH)x活性中心,可以高效催化醛、氨水和过氧化氢经一锅串联反应直接制备得到伯酰胺.A new microporous/mesoporous composite with a core-shell structure,TS-1@KCC-1,was fabri- cated in a microemulsion system by coating flower-like mesoporous silica(KCC-1) on the crystal surface of TS-1 zeolite.The synthesis conditions and a possible formation mechanism were studied in detail for the TS-1@KCC-1 material.A suitable temperature and assembly time were found to be 373–393 K and 4 h,respectively.The shell thickness of TS-1@KCC-1 was conveniently tuned in the range 25–80 nm.Rh(OH)x species were supported on TS-1@KCC-1,giving rise to a novel bifunc- tional tandem catalyst Rh(OH)x /TS-1@KCC-1,which effectively catalyzed the one-pot synthesis of primary amides directly from aldehydes,ammonia,and hydrogen peroxide.

关 键 词：TS-1分子筛 核壳材料 KCC-1 伯酰胺 串联催化剂 

分 类 号：O623.73[理学—有机化学]