Controlling coke deactivation and cracking selectivity of MFI zeolite by H3PO4 or KOH modification

被引：47
作者：
Epelde, Eva [1 ,2 ]
Santos, Jose I. [3 ]
Florian, Pierre [4 ,5 ]
Aguayo, Andres T. [1 ]
Gayubo, Ana G. [1 ]
Bilbao, Javier [1 ]
Castano, Pedro [1 ]
机构：
[1] Univ Basque Country UPV EHU, Dept Chem Engn, Bilbao 48080, Spain
[2] Univ Deusto, Fac Psychol & Educ, Dept Innovat & Sch Adm, Bilbao 48080, Spain
[3] Univ Basque Country UPV EHU, SGIKER, NMR Serv, San Sebastian 20018, Spain
[4] CNRS, UPR3079CEMHTI, F-45071 Orleans 2, France
[5] Univ Orleans, F-45067 Orleans 2, France
来源：
APPLIED CATALYSIS A-GENERAL | 2015年 / 505卷
关键词：
ZSM-5; zeolite; Acidity modification; Oligomerization-cracking; Propylene; Coke deactivation; INTENSIFYING PROPYLENE PRODUCTION; MODIFIED HZSM-5 CATALYST; PRODUCE LIGHT OLEFINS; SOLID-STATE NMR; ZSM-5; ZEOLITES; ACID SITES; MAS NMR; H-ZSM-5; TRANSFORMATION; 1-BUTENE;
D O I：
10.1016/j.apcata.2015.07.022
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：
The effect of the basic (KOH) or acid (H3PO4) treatment of the MFI (HZSM-5) zeolite has been studied comparing the structural and acidic features with the catalytic performance and deactivation of a set of unmodified and modified zeolites (SiO2/Al2O3 =30-280, 0-3 wt% of K or P). The properties of the catalysts have been elucidated using XRD, (27)AI and Si-29 NMR, N-2 adsorption-desorption, and adsorption-TPD of tert-butylamine. The catalytic performance has been evaluated in the cracking of 1-butene by means of initial, 5 h on-stream activity and coke formation. Our results point to the fact that using zeolites with high SiO2/Al2O3 ratio or neutralizing the strongest acid sites with KOH or H3PO4 increases propylene selectivity while decreases 1-butene conversion. The overall pathway of reaction involves propylene and other olefins as primary products that condensate in further steps to aromatics and ultimately to coke. This pathway can be controlled with less severe acidic features and by desilication with KOH or H3PO4 (particularly with the former). (C) 2015 The Authors. Published by Elsevier B.V.
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页码：105 / 115
页数：11
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