Mesoporous Zirconium Silicate Catalysts Prepared by Non-hydrolytic Acetamide Elimination

ŠKODA, David, Aleš STÝSKALÍK, Zdeněk MORAVEC and Jiří PINKAS. Mesoporous Zirconium Silicate Catalysts Prepared by Non-hydrolytic Acetamide Elimination. In 4th International Conference on Multifunctional, Hybrid and Nanomaterials, 9-13 March 2015 in Sitges, Spain, 2015. 2015.

Basic information

• Original name: Mesoporous Zirconium Silicate Catalysts Prepared by Non-hydrolytic Acetamide Elimination
• Authors: ŠKODA, David (203 Czech Republic, belonging to the institution), Aleš STÝSKALÍK (203 Czech Republic, belonging to the institution), Zdeněk MORAVEC (203 Czech Republic, belonging to the institution) and Jiří PINKAS (203 Czech Republic, guarantor, belonging to the institution).
• Edition: 4th International Conference on Multifunctional, Hybrid and Nanomaterials, 9-13 March 2015 in Sitges, Spain, 2015, 2015.

Other information

• Original language: English
• Type of outcome: Conference abstract
• Field of Study: 10402 Inorganic and nuclear chemistry
• Confidentiality degree: is not subject to a state or trade secret
• WWW: URL
• RIV identification code: RIV/00216224:14740/15:00083501
• Organization unit: Central European Institute of Technology
• Keywords in English: Zirconium silicate; Acetamide; Elimination; Nonhydrolytic; Mesoporous; Catalyst; Template

Abstract

Non-hydrolytic sol-gel reactions are efficient alternatives to classical aqueous techniques for synthesis of multimetallic oxides and inorganic-organic hybrid materials. This process provides better reaction control and higher homogeneity of prepared materials. We developed non-hydrolytic sol-gel routes to several groups of metallosilicate materials and efficient catalysts based on acetamide elimination reactions (1,2). Our approach is based on the acetamide condensation reaction of silicon tetraacetate Si(OAc)4 and zirconium diethylamide Zr(NEt2)4 that leads to the formation of Si–O–Zr bonds in the xerogel framework (IR, 29Si CPMAS NMR). Diethylacetamide and acetanhydride were confirmed (GC-MS, 1H NMR) as the reaction byproducts. To achieve the mesoporous nature of the xerogels, the reaction was successfully modified by the addition of the Pluronic P123 template with structure-directing and protecting functions which allow to prepare stiff gels. After heat treatment the template is burned out and xerogels are mesoporous with high surface areas. The presence of four-coordinated Zr atom introduces catalytic activity to our products. Calcined Si/Zr xerogels were tested in two types of catalytic reactions and the product yields were analyzed by GC-MS and 1H NMR. In the case of MPV reduction of 4-tert-butylcyclohexanone in 2-propanol the catalytic yield of 4-tert-butylcyclohexanone reached up to 55 % with a high selectivity for the trans product. Our Si/Zr xerogels are also very effective catalysts for aminolysis of styrene oxide with the 94 % conversion to catalytic products. The resulting xerogels and volatile byproducts were characterized by liquid and solid-state NMR, IR, GC-MS, surface area analysis, TGA, XRD and DRUV-Vis.

Links

• ED1.1.00/02.0068, research and development project: Name: CEITEC - central european institute of technology
• LH11028, research and development project: Name: Nehydrolytické sol-gelové reakce pro přípravu křemičitanů a fosforečnanů s řízenou porozitou a funkčními skupinami na povrchu (Acronym: NHSGKNOX)

Investor: Ministry of Education, Youth and Sports of the CR