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Two Synthesis Approaches of Fe-Containing Intercalated Montmorillonites: Differences as Acid Catalysts for the Synthesis of 1,5-Benzodeazepine from 1,2-Phenylenediamine and Acetone Full article

Journal Applied Clay Science
ISSN: 0169-1317 , E-ISSN: 1872-9053
Output data Year: 2017, Volume: 146, Pages: 388-396 Pages count : 9 DOI: 10.1016/j.clay.2017.06.028
Tags 1,2-Phenylenediamine, 1,5-Benzodiazepine, Cyclocondensation reaction, Fe,Al-pillared montmorillonite, Fe,Si-montmorillonite composites
Authors González Beatriz 1 , Trujillano Raquel 1 , Vicente Miguel A. 1 , Gil Antonio 2 , Panchenko Valentina N. 3,4 , Petrova Ekaterina A. 4 , Timofeeva Maria N. 3,4
Affiliations
1 Departamento de Química Inorgánica, Universidad de Salamanca, Salamanca, Spain
2 Departamento de Química Aplicada, Universidad Pública de Navarra, 31006 Pamplona, Spain
3 Boreskov Institute of Catalysis SB RAS, Prospekt Akad. Lavrentieva 5, 630090 Novosibirsk, Russian Federation
4 Novosibirsk State Technical University, Prospekt K. Marksa 20, 630092 Novosibirsk, Russian Federation

Funding (3)

1 Federal Agency for Scientific Organizations 0303-2016-0007
2 Ministry of Economic Affairs and Digital Transformation MAT2013-47811-C2-1-R, MAT2013-47811-C2-2-R
3 European Commission

Abstract: Two approaches were considered for the preparation of Fe-containing composites based on montmorillonite and comparison of their structural, physicochemical and catalytic properties. The first approach (Si,Fex-Mt materials) was based on the intercalation of Cheto montmorillonite (Mt) by 3-aminopropyltriethoxysilane (APTES) and FeCl3 via the sol-gel polymerization technique. Fe/Si atomic ratios were 6:94, 18:82 and 30:70. Then Si,Fex-Mt materials were calcined in air at 400 or 500ºC for the APTES removal. The second approach (Al13-xFex-Mt materials, x = 1 and 2) was based on the pillaring method using Keggin type mixed Al13-xFex-polycation (x = 1, 2) and montmorillonite from Cheto, Arizona, USA (Mt) as starting material. The intercalated Al13-xFex-Mt materials were calcined at 400 or 500ºC. The physicochemical characterization pointed out the effectiveness of the incorporation of Fe and Si into the interlayer space of the clay mineral. The fixation of small amounts of Fe (1.9 wt.%) increased the basal space from 9.57 to 13.89 Å, but the further fixation of Fe content slightly decreased the basal space. The specific surface area increased from 80 up to 171 m2/g. The oligomeric state of Fe2O3 particles depended on its content; the larger Fe content, the larger particle size of Fe2O3. Catalytic properties of Si,Fex-Mt and Al13-xFex-Mt materials were studied in the cyclocondensation of 1,2-phenylenediamine with acetone to 1,5-benzodiazepine. The yield of 1,5-benzodiazepine was found to rise with increasing of the Fe content in Si,Fex-Mt. Catalytic performance of Si,Fex-Mt was lower in comparison with Al13-xFex-Mt, that is in agreement with the amount of Lewis acid sites
Cite: González B. , Trujillano R. , Vicente M.A. , Gil A. , Panchenko V.N. , Petrova E.A. , Timofeeva M.N.
Two Synthesis Approaches of Fe-Containing Intercalated Montmorillonites: Differences as Acid Catalysts for the Synthesis of 1,5-Benzodeazepine from 1,2-Phenylenediamine and Acetone
Applied Clay Science. 2017. V.146. P.388-396. DOI: 10.1016/j.clay.2017.06.028 WOS Scopus РИНЦ AN OpenAlex
Dates:
Submitted: Apr 25, 2017
Accepted: Jun 24, 2017
Published online: Jun 29, 2017
Published print: Sep 15, 2017
Identifiers:
Web of science: WOS:000407655000049
Scopus: 2-s2.0-85030463259
Elibrary: 29740410
Chemical Abstracts: 2017:1109511
OpenAlex: W2725562925
Citing:
DB Citing
Web of science 12
Scopus 13
Elibrary 17
OpenAlex 16
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