Methanol to olefins: activity and stability of nanosized SAPO-34 molecular sieves and control of selectivity by silicon distribution

被引:119
|
作者
Li, Zhibin [1 ]
Martinez-Triguero, Joaquin [1 ]
Concepcion, Patricia [1 ]
Yu, Jihong [2 ]
Corma, Avelino [1 ]
机构
[1] Univ Politecn Valencia, Inst Tecnol Quim, CSIC, Valencia 46022, Spain
[2] Jilin Univ, Coll Chem, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130021, Peoples R China
基金
中国国家自然科学基金;
关键词
MESOPOROUS SSZ-13 ZEOLITE; SOLID-STATE NMR; CATALYTIC PERFORMANCE; SILICOALUMINOPHOSPHATES H-SAPO-34; THERMAL-STABILITY; COKE DEPOSITION; MIXED TEMPLATE; COMBINED FTIR; MTO REACTION; CONVERSION;
D O I
10.1039/c3cp52247d
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
Nano-SAPO-34 molecular sieves synthesized in a microwave environment with 20 nm crystal size showed a longer lifetime than SAPO-34 prepared by the conventional hydrothermal method in the reaction of methanol to olefins. It has been found that silicon distribution strongly affects the lifetime and selectivity. Thus, silicon at the border of the silicon islands gives a higher lifetime and lower C2/C3 ratio. This change in activity and selectivity is better explained in terms of different silicon distribution than by preferential diffusion of ethene through the 8MR pores and agrees with transition-state selectivity. The effects of equilibrium of olefins and deactivation by coke were isolated, showing that after full formation of the hydrocarbon pool, selectivity is independent of deactivation by coke.
引用
收藏
页码:14670 / 14680
页数:11
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