Synthesis of hierarchical nanocrystalline β zeolite as efficient catalyst for alkylation of benzene with benzyl alcohol.
Synthesis of hierarchical nanocrystalline β zeolite as efficient catalyst for alkylation of benzene with benzyl alcohol.
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DOI：
10.1039/d2ra00209d
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发表时间：
2022-02-03
期刊：
影响因子：
3.9
通讯作者：
Hao QQ
中科院分区：
文献类型：
--
作者：
Zhou P;Liu MN;Luo QX;Zhang J;Chen H;Ma X;Hao QQ
为了开发一种高效的固体酸催化剂用于Friedel-Crafts烷基化反应，特别是涉及大分子的烷基化反应，采用两亲性有机硅烷[（CH 3 O）3SiC 3 H6 N（CH 3）2C 18 H37]Cl，TPOAC作为协同结构导向剂（SDA），直接合成了分级结构纳米晶β沸石。详细研究了β沸石的生长过程以及TPOAC/SiO2摩尔比对β沸石介孔结构、晶粒尺寸和酸性的影响。表征结果表明，在分级β沸石上通过β纳米晶的堆积形成了晶内介孔和晶间介孔/大孔。与常规微孔β沸石相比，大部分强酸中心得到了很好的保留。结果表明，在优化的合成条件下合成的分级结构纳米晶β沸石在苯与苯甲醇烷基化反应中表现出了更高的酸中心比催化活性（转换数TON），这是由于分级结构β沸石具有良好的介孔性、酸中心可及性和强酸中心的综合平衡.采用两亲性有机硅烷表面活性剂作为介孔导向剂和晶体生长抑制剂，制备了具有高传递性和高催化活性的多级结构β沸石。
To develop an efficient solid acid catalysts for the Friedel–Crafts alkylation reaction, especially for involving bulky molecules, the direct synthesis of hierarchical nanocrystalline β zeolites were achieved by using amphiphilic organosilane ([(CH3O)3SiC3H6N(CH3)2C18H37]Cl, TPOAC) as collaborative structure-directing agent (SDA). The growth evolution of β crystals and the influence of TPOAC/SiO2 molar ratio on the mesoporous structure, crystal size, and acidic properties of β zeolites were investigated and discussed in detail. The characterization results reveal that intracrystalline mesopores and intercrystalline mesopores/macropores via the stacking of β nanocrystals were generated over the hierarchical β zeolites. Moreover, most of the strong acid sites were well remained compared with the conventional microporous β zeolite. Consequently, the hierarchical nanocrystalline β zeolite synthesized under the optimized synthesis conditions shows improved specific catalytic activity of acid sites (turnover number, TON) in alkylation of benzene with benzyl alcohol, which can be attributed to the integrated balance of considerable mesoporosity, accessibility of the acid sites, and well-remained strong acid sites in the hierarchical β zeolite. Hierarchical β zeolite with enhanced transport and specific catalytic activity of acid sites in Friedel–Crafts alkylation was achieved by using amphiphilic organosilane surfactant as mesopores-directing agent and crystal growth inhibitor.
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