The present study reports a novel strategy to fabricate nanocrystal-assembled hierarchical MOR zeolites. This is the first demonstration of hierarchical MOR without preferential growth along the c-axis, which facilita...The present study reports a novel strategy to fabricate nanocrystal-assembled hierarchical MOR zeolites. This is the first demonstration of hierarchical MOR without preferential growth along the c-axis, which facilitates mass transfer in the 12-membered ring channels of MOR zeolite for the conversions involving bulky molecules. The facile method involves the combined use of tetraethylammonium hydroxide （TEAOH） and commercial surfactants, in which TEAOH is essential for the construction of nanocrystal assemblies. The surfactant serves as a crystal growth-inhibiting agent to further inhibit nanocrystalline particle growth, resulting in enhanced mesoporosity. The hierarchical MOR assembled particles, constructed of 20-50-nm crystallites, exhibit superior catalytic properties in the alkylation of benzene with benzyl alcohol compared with the control sample, as the hierarchical MOR possesses a larger external surface area and longer c-axis dimension. More importantly, the material shows improved activity and stability in the dimethyl ether carbonylation to methyl acetate reaction, which is a novel route to produce ethanol from syngas.展开更多
Well-crystallized zeolite beta was synthesized by using acid-leached metakaolin as the silica-alumina source and tetraethylammonium hydroxide structure-directing agent.The influence of the composition of the reaction ...Well-crystallized zeolite beta was synthesized by using acid-leached metakaolin as the silica-alumina source and tetraethylammonium hydroxide structure-directing agent.The influence of the composition of the reaction mixture on product crystallinity was investigated,and the crystallization process was studied by examining solid samples obtained at different synthesis times.Results showed that the acid-leached metakaolin was fully converted into soluble aluminum and silicon species,which is crucial for the formation of well-crystallized zeolite beta.At the beginning of the crystallization process,these soluble aluminum and silicon species formed a aluminum-rich intermediate structure with layer morphology.With the crystallization proceeding,more silicon species were incorporated into the zeolite beta framework and the layered structure was changed into spherical particles of zeolite beta with high SiO 2 /Al 2 O 3 ratio and crystallinity.展开更多
基金supported by the National Natural Science Foundation of China(21101150,21476228,21473182)~~
文摘The present study reports a novel strategy to fabricate nanocrystal-assembled hierarchical MOR zeolites. This is the first demonstration of hierarchical MOR without preferential growth along the c-axis, which facilitates mass transfer in the 12-membered ring channels of MOR zeolite for the conversions involving bulky molecules. The facile method involves the combined use of tetraethylammonium hydroxide （TEAOH） and commercial surfactants, in which TEAOH is essential for the construction of nanocrystal assemblies. The surfactant serves as a crystal growth-inhibiting agent to further inhibit nanocrystalline particle growth, resulting in enhanced mesoporosity. The hierarchical MOR assembled particles, constructed of 20-50-nm crystallites, exhibit superior catalytic properties in the alkylation of benzene with benzyl alcohol compared with the control sample, as the hierarchical MOR possesses a larger external surface area and longer c-axis dimension. More importantly, the material shows improved activity and stability in the dimethyl ether carbonylation to methyl acetate reaction, which is a novel route to produce ethanol from syngas.
基金supported by Beijing Natural Science Foundation (Grant No.2093043)the National Natural Science Foundation of China (Grant No.20606038)
文摘Well-crystallized zeolite beta was synthesized by using acid-leached metakaolin as the silica-alumina source and tetraethylammonium hydroxide structure-directing agent.The influence of the composition of the reaction mixture on product crystallinity was investigated,and the crystallization process was studied by examining solid samples obtained at different synthesis times.Results showed that the acid-leached metakaolin was fully converted into soluble aluminum and silicon species,which is crucial for the formation of well-crystallized zeolite beta.At the beginning of the crystallization process,these soluble aluminum and silicon species formed a aluminum-rich intermediate structure with layer morphology.With the crystallization proceeding,more silicon species were incorporated into the zeolite beta framework and the layered structure was changed into spherical particles of zeolite beta with high SiO 2 /Al 2 O 3 ratio and crystallinity.
