Restraining deactivation of ?-zeolite by modifying with MgAl2O4 spinel in

被引:12
作者
de Oliveira, Amanda Sayure Kasuya [1 ]
Lopes, Antonio Marcelo Silva [1 ]
Barbosa, Felipe Fernandes [1 ]
da Silva, Francisco Ivan [3 ,4 ]
de Sousa, Jose Antonio [3 ]
Pontes, Luiz Antonio Magalhaes [2 ]
Pergher, Sibele B. C. [1 ]
Braga, Tiago Pinheiro [1 ]
机构
[1] Univ Fed Rio Grande do Norte, Lab Peneiras Mol LABPEMOL, Inst Quim, BR-59078970 Natal, RN, Brazil
[2] Univ Fed Bahia, Postgrad Program Chem Engn, St Prof Aristides Novis 2,Federaca, BR-40210630 Salvador, BA, Brazil
[3] Fed Inst Piaui, IFPI, Rodovia BR 407, BR-64750000 Paulistana, PI, Brazil
[4] Univ Fed Piaui UFPI, Campus Univ Minist Petronio Portella Ininga, BR-64049550 Teresina, PI, Brazil
关键词
-zeolite; Restraining deactivation; Glycerol; Acrolein; GAS-PHASE DEHYDRATION; GLYCEROL DEHYDRATION; MGAL2O4; SPINEL; BETA ZEOLITES; ALLYL ALCOHOL; ACRYLIC-ACID; H-BETA; CATALYSTS; ACROLEIN; CONVERSION;
D O I
10.1016/j.mcat.2022.112414
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
MgAl2O4 dispersed on HBEA zeolite with different spinel contents were successfully synthesized and their glycerol dehydration performances were presented. The different solids were characterized by XRD, infrared (IR) and Raman spectroscopy, N2 physisorption, SEM-FEG, acidity by TPD-NH3 and DRIFTS-pyridine adsorption. It was not possible to observe the spinel phase in the diffractograms due to its high dispersion, while the reflections of the HBEA were evidenced in the different samples. The Raman and infrared spectra suggested the presence of stretches concerning the MgAl2O4 spinel. N2 isotherms and low-angle XRD indicated that the pore structure and textural properties were altered after impregnation, but the micro-mesoporosity of zeolite was maintained. The HBEA morphology did not undergo significant changes by modification with spinel and the metals are evenly distributed according to SEM and EDS spectral mapping. The addition of spinel on zeolite caused a change in the acidic properties of HBEA related to the type, number and strength of the sites according to the TPD profiles and the DRIFTS spectra. The 2% of MgAl2O4 on HBEA catalyst exhibited the best catalytic performance due to the effects of its acidic and textural properties, reaching 60% of glycerol conversion, 66% of acrolein selectivity in 6 h and 16% of coke deposited in 10 h, restricting deactivation compared to pure zeolite. The reaction pathway for the different products formed depending on the type of acid site were detailed in the proposed mechanism and correlated with electrostatic potential maps as well as the reactions for coke formation were described according to compounds identified by GC-MS after coke extraction.
引用
收藏
页数:16
相关论文
共 68 条
[1]   Direct conversion of methane to C2 hydrocarbons using W supported on sulfated zirconia solid acid catalyst [J].
Abedin, Md Ashraful ;
Bhattar, Srikar ;
Spivey, James J. .
SN APPLIED SCIENCES, 2020, 2 (12)
[2]   Gas-phase conversion of glycerol to allyl alcohol over vanadium-supported zeolite beta [J].
Alineida, Ruben ;
Filipa Ribeiro, M. ;
Fernandes, Auguste ;
Lourenco, Joao P. .
CATALYSIS COMMUNICATIONS, 2019, 127 :20-24
[3]   Oxidative dehydrogenation of ethylbenzene to styrene over the CoFe2O4-MCM-41 catalyst: preferential adsorption on the O2-Fe3+O2- sites located at octahedral positions [J].
Borges Soares, Mosses da Costa ;
Barbosa, Felipe Fernandes ;
Morales Torres, Marco Antonio ;
Valentini, Antoninho ;
Albuquerque, Anderson dos Reis ;
Sambrano, Julio Ricardo ;
Pergher, Sibele B. C. ;
Essayem, Nadine ;
Braga, Tiago Pinheiro .
CATALYSIS SCIENCE & TECHNOLOGY, 2019, 9 (10) :2469-2484
[4]   Determination of the catalytically active oxidation Lewis acid sites in Sn-beta zeolites, and their optimisation by the combination of theoretical and experimental studies [J].
Boronat, M ;
Concepción, P ;
Corma, A ;
Renz, M ;
Valencia, S .
JOURNAL OF CATALYSIS, 2005, 234 (01) :111-118
[5]   Efficiency of zeolite MCM-22 with different SiO2/Al2O3 molar ratios in gas phase glycerol dehydration to acrolein [J].
Carrico, Camila S. ;
Cruz, Fernanda T. ;
Santos, Mauricio B. ;
Pastore, Heloise O. ;
Andrade, Heloysa M. C. ;
Mascarenhas, Artur J. S. .
MICROPOROUS AND MESOPOROUS MATERIALS, 2013, 181 :74-82
[6]   Progress of the Catalytic Deactivation of H-ZSM-5 Zeolite in Glycerol Dehydration [J].
Catuzo, Gabriel L. ;
Possato, Luiz G. ;
Sad, Maria Eugenia ;
Padro, Cristina ;
Martins, Leandro .
CHEMCATCHEM, 2021, 13 (20) :4419-4430
[7]   Glycerol dehydration to hydroxyacetone in gas phase over copper supported on magnesium oxide (hydroxide) fluoride catalysts [J].
Celerier, Stephane ;
Morisset, Sophie ;
Batonneau-Gener, Isabelle ;
Belin, Thomas ;
Younes, Khaled ;
Batiot-Dupeyrat, Catherine .
APPLIED CATALYSIS A-GENERAL, 2018, 557 :135-144
[8]   CATALYTIC ACTIVITY OF LARGE-PORE HIGH SI/AL ZEOLITES - CRACKING OF HEPTANE ON H-BETA AND DEALUMINATED HY ZEOLITES [J].
CORMA, A ;
FORNES, V ;
MONTON, JB ;
ORCHILLES, AV .
JOURNAL OF CATALYSIS, 1987, 107 (02) :288-295
[9]   Metal-Exchanged β Zeolites as Catalysts for the Conversion of Acetone to Hydrocarbons [J].
Cruz-Cabeza, Aurora J. ;
Esquivel, Dolores ;
Jimenez-Sanchidrian, Cesar ;
Romero-Salguero, Francisco J. .
MATERIALS, 2012, 5 (01) :121-134
[10]   Raman fingerprint of chromate, aluminate and ferrite spinels [J].
D'Ippolito, Veronica ;
Andreozzi, Giovanni B. ;
Bersani, Danilo ;
Lottici, Pier Paolo .
JOURNAL OF RAMAN SPECTROSCOPY, 2015, 46 (12) :1255-1264