Acidity and Characterization of 12-Tungstophosphoric Acid Supported on Silica-Alumina

被引:28
作者
de Mattos, Flavia C. G. [1 ]
de Carvalho, Eduardo N. C. B. [1 ]
de Freitas, Elon F. [1 ]
Paiva, Mateus F. [1 ]
Ghesti, Grace F. [1 ]
de Macedo, Julio L. [1 ]
Dias, Silvia C. L. [1 ]
Dias, Jose A. [1 ]
机构
[1] Univ Brasilia, Inst Quim, Lab Catalise, Campus Darcy Ribeiro,CP 4478, BR-70904970 Brasilia, DF, Brazil
关键词
supported heteropolyacid; 12-tungstophosphoric acid; silica-alumina; ethanol; esterification of acetic acid with ethanol; LIQUID-PHASE ESTERIFICATION; HETEROPOLY ACIDS; ACETIC-ACID; REACTION-KINETICS; GAS-PHASE; H3PW12O40; CATALYST; SITES; NMR; IMMOBILIZATION;
D O I
10.5935/0103-5053.20160183
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
This work deals with preparation and characterization of H3PW12O40 (H3PW) supported on silica-alumina. Impregnation of H3PW (15, 20, 30 and 40 wt.%) on commercial silica-alumina support in acidic aqueous solution is effective for preparing this catalyst keeping its Keggin structure, according to different methods of characterization. The catalysts were tested in a model reaction of acetic acid with ethanol and 30 wt.% H3PW/SiO2-Al2O3 had the highest activity under the conditions: catalyst calcination at 300 degrees C, temperature of 100 degrees C, acetic acid: ethanol molar ratio of 2: 1 and catalyst: acetic acid mass ratio of 10 wt.%. The reaction yield was 79 and 100% selectivity for ethyl acetate over three reutilizations, for reaction time of 2 h. The calculated total acid site distribution was 0.299 mmol g(-1) (97% of the theoretical probed by pyridine), and most of these (0.236 mmol g(-1)) were Bronsted weak-medium strength (pyridine desorption between 300 and 500 degrees C).
引用
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页码:336 / +
页数:19
相关论文
共 60 条
[1]   Improved method for immobilization of a chiral complex on PTA/alumina for asymmetric hydrogenation of a β-ketoester [J].
Ahn, Sung-Hyun ;
Choi, Moo-Seok ;
Im, Jun-Seop ;
Sheikh, Rizwan ;
Park, Yeung-Ho .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2013, 373 :55-60
[2]   Heteropoly acids as catalysts for liquid-phase esterification and transesterification [J].
Alsalme, Ali ;
Kozhevnikova, Elena F. ;
Kozhevnikov, Ivan V. .
APPLIED CATALYSIS A-GENERAL, 2008, 349 (1-2) :170-176
[3]   Anchored homogeneous catalysts: the role of the heteropoly acid anchoring agent [J].
Augustine, RL ;
Tanielyan, SK ;
Mahata, N ;
Gao, Y ;
Zsigmond, A ;
Yang, H .
APPLIED CATALYSIS A-GENERAL, 2003, 256 (1-2) :69-76
[4]   Esterification of Acetic Acid with n-Butanol Using Heteropoly Acid Supported Modified Clay Catalyst [J].
Bhorodwaj, Siddhartha Kumar ;
Pathak, Madan Gopal ;
Dutta, Dipak Kumar .
CATALYSIS LETTERS, 2009, 133 (1-2) :185-191
[5]   Heteropolyacid supported on montmorillonite catalyst for dehydration of dilute bio-ethanol [J].
Bokade, Vijay V. ;
Yadav, Ganapati D. .
APPLIED CLAY SCIENCE, 2011, 53 (02) :263-271
[6]   Intramolecular cyclization of (+)-citronellal using supported 12-tungstophosphoric acid on MCM-41 [J].
Braga, Patricia R. S. ;
Costa, Andreia A. ;
de Freitas, Elon F. ;
Rocha, Rafael O. ;
de Macedo, Julio L. ;
Araujo, Antonio S. ;
Dias, Jose A. ;
Dias, Silvia C. L. .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2012, 358 :99-105
[7]   Catalyst materials based on Nb2O5 supported on SiO2-Al2O3:: Preparation and structural characterization [J].
Braga, VS ;
Dias, JA ;
Dias, SCL ;
de Macedo, JL .
CHEMISTRY OF MATERIALS, 2005, 17 (03) :690-695
[8]   DODECATUNGSTOPHOSPHORIC ACID HEXAHYDRATE, (H5O2+)3(PW12O403-) - TRUE STRUCTURE OF KEGGINS PENTAHYDRATE FROM SINGLE-CRYSTAL X-RAY AND NEUTRON-DIFFRACTION DATA [J].
BROWN, GM ;
NOESPIRLET, MR ;
BUSING, WR ;
LEVY, HA .
ACTA CRYSTALLOGRAPHICA SECTION B-STRUCTURAL SCIENCE CRYSTAL ENGINEERING AND MATERIALS, 1977, 33 (APR15) :1038-1046
[9]   Solvent effect on the preparation of H3PW12O40 supported on alumina [J].
Caliman, E ;
Dias, JA ;
Dias, SCL ;
Prado, AGS .
CATALYSIS TODAY, 2005, 107-08 :816-825
[10]   Preparation and characterization of H3PW12O40 supported on niobia [J].
Caliman, Edneia ;
Dias, Jose A. ;
Dias, Silvia C. L. ;
Garcia, Fillipe A. C. ;
de Macedo, Julio L. ;
Almeida, Liana S. .
MICROPOROUS AND MESOPOROUS MATERIALS, 2010, 132 (1-2) :103-111