晶种辅助的硅硼硅镓沸石分子筛的硅铝催化功能化

硅铝酸盐分子筛是最早发现的一个沸石分子筛亚类。由于其具有天然可调的酸性，使其成为催化功能最丰富的一类分子筛。但在现有245种分子筛中，有130余种分子筛不能实现硅铝酸盐形式。从而大大限制了这一部分分子筛的催化应用。其中，硅硼酸盐和硅镓酸盐和硅铝酸盐结构组成最相近。在现有报道中，人们主要通过后处理铝插入的方法实现这一部分分子筛的硅铝酸盐形式的合成。但是这种方法也存在明显的缺陷，1）B，Ga等杂原子在某些情况下不能完全脱除；2）酸处理过程中影响结晶度；3）在补铝的过程中会有非骨架铝残留；4）骨架中的缺陷没有完全被铝填补；5）过程复杂等。基于上述原因，需要探索新的路线实现非硅铝酸盐的硅铝化。本项目中，申请者主要针对一系列硅硼硅镓酸盐分子筛，探索使用晶种辅助直接合成的方法实现该系列分子筛的硅铝酸盐催化功能化。并对晶种进行深入的晶面分析，计算晶种晶面能，从而指导晶种的晶貌控制和硅铝酸盐功能化合成。

Aluminosilicate is earliest found subgroup of zeolite. The naturally occurred acid sites render it as a most catalytic powerful zeolite. However, among the 245 type of zeolite by International Zeolite Association, more than 130 types of zeolite are not yet realized in aluminosilicate form, thus impede their catalytic applications. Due to the structure chemistry similarity, borosilicate and Gallosilicate are most aluminosilicate relevant. To our best knowledge, the boro/gallosilicate zeolite could be transform into aluminosilicate form in post-synthesis treatment, i.e. Al-reinsertion. Nevertheless, the post treatment are strongly limited by the issues: 1) B and Ga are not completely removable. 2) Crystallinity may be irreversibly decreased during the acid treatment. 3) Octahedral coordinated Al spices may residue in the zeolite channel while 4) some defects are not amended. 5 The process is complicate. Thus a set of aluminosilicate zeolite form is suggested being realizable from coresponding boro/gallosilicate in this proposal. That is to direct synthesis aluminosilicate form using the boro/gallosilicate seed assisted method. Furthermore, the seed crystal face energy analysis by theoretical calculation will be performed once the seed is obtained. Hence, the insight understanding of seed assisted zeolite synthesis is achieved besides the a couple of boro/gallosilicate zeolite been transformed into aluminosilicate.