Synthesis and Catalytic Properties of Metal Clusters Encapsulated within Small-Pore (SOD, GIS, ANA) Zeolites

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• 作者：Sarika Goel ; Zhijie Wu ; Stacey I. Zones ; Enrique Iglesia
• 刊名：The Journal of the American Chemical Society
• 出版年：2012
• 出版时间：October 24, 2012
• 年：2012
• 卷：134
• 期：42
• 页码：17688-17695
• 全文大小：454K
• 年卷期：v.134,no.42(October 24, 2012)
• ISSN：1520-5126

文摘

The synthesis protocols for encapsulation of metal clusters reported here expand the diversity in catalytic chemistries made possible by the ability of microporous solids to select reactants, transition states, and products on the basis of their molecular size. We report a synthesis strategy for the encapsulation of noble metals and their oxides within SOD (Sodalite, 0.28 nm 脳 0.28 nm), GIS (Gismondine, 0.45 nm 脳 0.31 nm), and ANA (Analcime, 0.42 nm 脳 0.16 nm) zeolites. Encapsulation was achieved via direct hydrothermal synthesis for SOD and GIS using metal precursors stabilized by ammonia or organic amine ligands, which prevent their decomposition or precipitation as colloidal hydroxides at the conditions of hydrothermal synthesis (<380 K) and favor interactions between metal precursors and incipient aluminosilicate nuclei during self-assembly of microporous frameworks. The synthesis of ANA requires higher crystallization temperatures (415 K) and high pH (>12), thereby causing precipitation of even ligand-stabilized metal precursors as hydroxides. As a result, encapsulation was achieved by the recrystallization of metal clusters containing GIS into ANA, which retained these metal clusters within voids throughout the GIS鈥揂NA transformation.