负载型铜系分子筛催化剂在苯酚羟基化反应中的应用

Application of Molecular Sieve-supported Copper Catalysts in Hydroxylation of Phenol

以介孔分子筛MCM-41、MCM-48和AlMCM-41以及微孔分子筛Naβ和MOR为载体,分别采用有机官能团化法和分步水热合成法制备了系列负载型催化剂,考察了其在苯酚羟基化反应中的活性;得到了不同载体类型、不同负载方法及不同助剂与反应活性的对应关系.结果表明:以微孔分子筛为载体的催化剂对副产物有明显的抑制作用.介孔分子筛AlMCM-41,MCM-41,MCM-48为载体时,催化剂在苯酚羟基化反应中的活性顺序为AlMCM-41>MCM-48>MCM-41,助剂镧和钴的引入可以有效抑制副产物的产生.

In the present research, a series supporting catalysts were prepared by the stepped hydrothermal and organofunctionalization methods, in which mesoporous molecular sieves MCM-41, MCM-48, AlMCM-41 and microporous molecular sieves Naβ and MOR were respectively employed as supports. Activities of various kinds of cata- lysts in hydroxylation of phenol were investigated, the influence on activity by different supports and loading methods and promoter were also studied. It was resulted that microporous molecular sieve supporting active composition catalysts showed apparently inhibiting action to by-products. The sequence of activities in hydroxylation of phenol was A1MCM-41 〉 MCM-48 〉 MCM-41 when employed mesoporous molecular sieve AlMCM-41, MCM-41, MCM-48 as supports. Besides, the by-products were remarkably reduced when La and Co was introduced as promoter.