Mesoporous Zirconium Silicate Catalysts Prepared by
Non-hydrolytic Acetamide Elimination

a 2015

Mesoporous Zirconium Silicate Catalysts Prepared by Non-hydrolytic Acetamide Elimination

ŠKODA, David, Aleš STÝSKALÍK, Zdeněk MORAVEC a Jiří PINKAS

Základní údaje

Originální název

Mesoporous Zirconium Silicate Catalysts Prepared by Non-hydrolytic Acetamide Elimination

Autoři

ŠKODA, David (203 Česká republika, domácí), Aleš STÝSKALÍK (203 Česká republika, domácí), Zdeněk MORAVEC (203 Česká republika, domácí) a Jiří PINKAS (203 Česká republika, garant, domácí)

Vydání

4th International Conference on Multifunctional, Hybrid and Nanomaterials, 9-13 March 2015 in Sitges, Spain, 2015, 2015

Další údaje

Jazyk

angličtina

Typ výsledku

Konferenční abstrakt

Obor

10402 Inorganic and nuclear chemistry

Utajení

není předmětem státního či obchodního tajemství

Odkazy

URL

Kód RIV

RIV/00216224:14740/15:00083501

Organizační jednotka

Středoevropský technologický institut

Klíčová slova anglicky

Zirconium silicate; Acetamide; Elimination; Nonhydrolytic; Mesoporous; Catalyst; Template

Změněno: 18. 3. 2016 18:03, prof. RNDr. Jiří Pinkas, Ph.D.

Anotace

V originále

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.

Návaznosti

ED1.1.00/02.0068, projekt VaV

Název: CEITEC - central european institute of technology

LH11028, projekt VaV

Název: Nehydrolytické sol-gelové reakce pro přípravu křemičitanů a fosforečnanů s řízenou porozitou a funkčními skupinami na povrchu (Akronym: NHSGKNOX)

Investor: Ministerstvo školství, mládeže a tělovýchovy ČR, Nehydrolytické sol-gelové reakce pro přípravu křemičitanů a fosforečnanů s řízenou porozitou a funkčními skupinami na povrchu

Citovat

ŠKODA, David, Aleš STÝSKALÍK, Zdeněk MORAVEC a 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.

@proceedings{1307897,
   author = {Škoda, David and Stýskalík, Aleš and Moravec, Zdeněk and Pinkas, Jiří},
   booktitle = {4th International Conference on Multifunctional, Hybrid and Nanomaterials, 9-13 March 2015 in Sitges, Spain, 2015},
   keywords = {Zirconium silicate; Acetamide; Elimination; Nonhydrolytic; Mesoporous; Catalyst; Template},
   language = {eng},
   title = {Mesoporous Zirconium Silicate Catalysts Prepared by Non-hydrolytic Acetamide Elimination},
   url = {http://www.hybridmaterialsconference.com/},
   year = {2015}
}

TY  - CONF
ID  - 1307897
AU  - Škoda, David - Stýskalík, Aleš - Moravec, Zdeněk - Pinkas, Jiří
PY  - 2015
TI  - Mesoporous Zirconium Silicate Catalysts Prepared by Non-hydrolytic Acetamide Elimination
KW  - Zirconium silicate
KW  - Acetamide
KW  - Elimination
KW  - Nonhydrolytic
KW  - Mesoporous
KW  - Catalyst
KW  - Template
UR  - http://www.hybridmaterialsconference.com/
L2  - http://www.hybridmaterialsconference.com/
N2  - 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.
ER  -

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

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