Role of Zn-Al oxide structure and oxygen vacancy in bifunctional catalyst for syngas conversion to light olefins

被引:7
|
作者
Meng, Fanhui [1 ]
Li, Baozhen [1 ]
Zhang, Jinghao [1 ]
Wang, Lina [1 ]
Li, Zhong [1 ]
机构
[1] Taiyuan Univ Technol, State Key Lab Clean & Efficient Coal Utilizat, Taiyuan 030024, Peoples R China
关键词
ZnAl; 2; O; 4; spinel; Precipitation; Metal oxide structure; Oxygen vacancy; Syngas; Light olefins; SELECTIVITY; NI;
D O I
10.1016/j.fuel.2023.128351
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
Metal oxide plays a vital role in bifunctional tandem-catalyzed CO hydrogenation to light olefins. Herein, a series of Zn-Al metal oxides were prepared and then physically mixed with SAPO-18, the prepared bifunctional catalyst was applied in direct conversion of syngas to light olefins. The effects of structure and oxygen vacancy of Zn-Al oxide were studied by changing the preparation method and the sequence of precipitation. The sequentialprecipitated ZA-SP oxide exhibits the ZnAl2O4 spinel structure and no obvious crystalline phase of gamma-Al2O3 or ZnO. Compared with the reverse- or co-precipitated or the impregnated Zn-Al oxides, ZA-SP oxide possesses the highest oxygen vacancy content and amounts of desorbed CO, which facilitates the CO adsorption and activation. The adsorbed and activated CO on the surface of Zn-Al oxide converted to *CH3O intermediates with the dissociated H species on -Zn-O- sites, and then formed reaction intermediates as in methanol to olefins reaction. After optimizing the calcination temperature of ZA-SP oxide, weight ratio of ZA-SP to SAPO-18, reaction temperature, and gas hourly space velocity, the ZA-SP/SAPO-18 bifunctional catalyst exhibits the highest light olefins space time yield of 10.0 mmol center dot gcat- 1 center dot h- 1 at a CO conversion of 40.2 %, which outperforms the previous reported values.
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页数:11
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