Effect of preparation methods on the structure and catalytic performance of Fe-Zn/K catalysts for CO2 hydrogenation to light olefins

doi:10.1016/j.cjche.2017.10.013

Chinese Journal of Chemical Engineering ›› 2018, Vol. 26 ›› Issue (4): 761-767.DOI: 10.1016/j.cjche.2017.10.013

• Catalysis, Kinetics and Reaction Engineering • 上一篇下一篇

Effect of preparation methods on the structure and catalytic performance of Fe-Zn/K catalysts for CO₂ hydrogenation to light olefins

Xu Wang, Jianli Zhang, Jingyu Chen, Qingxiang Ma, Subing Fan, Tiansheng Zhao

State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, College of Chemistry & Chemical Engineering, Ningxia University, Yinchuan 750021, China

收稿日期:2017-07-27 修回日期:2017-10-31 出版日期:2018-04-28 发布日期:2018-05-19
通讯作者: Jianli Zhang,E-mail addresses:zhangjl@nxu.edu.cn;Tiansheng Zhao,E-mail addresses:zhaots@nxu.edu.cn
基金资助:
Supports by the National Natural Science Foundation of China (21666030, 21366025) and National First-rate Discipline Construction Project of Ningxia (NXYLXK2017A04).

Effect of preparation methods on the structure and catalytic performance of Fe-Zn/K catalysts for CO₂ hydrogenation to light olefins

Xu Wang, Jianli Zhang, Jingyu Chen, Qingxiang Ma, Subing Fan, Tiansheng Zhao

State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, College of Chemistry & Chemical Engineering, Ningxia University, Yinchuan 750021, China

Received:2017-07-27 Revised:2017-10-31 Online:2018-04-28 Published:2018-05-19
Contact: Jianli Zhang,E-mail addresses:zhangjl@nxu.edu.cn;Tiansheng Zhao,E-mail addresses:zhaots@nxu.edu.cn
Supported by:
Supports by the National Natural Science Foundation of China (21666030, 21366025) and National First-rate Discipline Construction Project of Ningxia (NXYLXK2017A04).

摘要/Abstract

摘要： Potassium promoted iron-zinc catalysts prepared by co-precipitation method (C-Fe-Zn/K), solvothermal method (S-Fe-Zn/K) and hydrothermal method (H-Fe-Zn/K) could selectively convert CO₂ to light olefins, respectively. The physicochemical properties of the obtained catalysts were determined by SEM, N₂ physisorption, XRD, H₂-TPR, CO₂-TPD and XPS measurements. The results demonstrated that preparation methods had great influences on the morphology, phase structures, reduction and adsorption behavior, and hence the catalytic performance of the catalysts. The samples prepared by hydrothermal and co-precipitation method generated small uniform particles and led to lower specific surface area. In contrast, microspheres with larger specific surface area were formed by self-assembly of nanosheets using solvothermal method. ZnFe₂O₄ was the only detectable phase in the fresh C-2Fe-1Zn/K, S-3Fe-1Zn/K and S-2Fe-1Zn/K samples. ZnFe₂O₄ and ZnO co-existed with increasing Zn content in S-1Fe-1Zn/K sample, while ZnO and Fe₂O₃ could be observed over H-2Fe-1Zn/K sample. All the used samples contained Fe3O4, ZnO and Fe₅C₂. The peak intensity of ZnO was strong in the AR-H-2Fe-1Zn/K sample while it was the lowest in the AR-C-2Fe-1Zn/K sample after reaction. The formation of ZnFe₂O₄ increased the interaction between iron and zinc for C-2Fe-1Zn/K and S-Fe-Zn/K samples, causing easier reduction of Fe₂O₃ to Fe3O4. The surface basicity of the sample prepared by co-precipitation method was much more than that of the other two methods. During CO₂ hydrogenation, all the catalysts showed good activity and olefin selectivity. The CO selectivity was increased with increasing Zn content over S-Fe-Zn/K samples. H-2Fe-1Zn/K catalyst preferred to the production of C₅⁺ hydrocarbons. CO₂ conversion of 54.76% and C₂⁼-C₄⁼ contents of 57.38% were obtained on C-2Fe-1Zn/K sample, respectively.

关键词: CO₂ hydrogenation, Light olefins, Preparation methods, Iron-zinc catalyst

Abstract: Potassium promoted iron-zinc catalysts prepared by co-precipitation method (C-Fe-Zn/K), solvothermal method (S-Fe-Zn/K) and hydrothermal method (H-Fe-Zn/K) could selectively convert CO₂ to light olefins, respectively. The physicochemical properties of the obtained catalysts were determined by SEM, N₂ physisorption, XRD, H₂-TPR, CO₂-TPD and XPS measurements. The results demonstrated that preparation methods had great influences on the morphology, phase structures, reduction and adsorption behavior, and hence the catalytic performance of the catalysts. The samples prepared by hydrothermal and co-precipitation method generated small uniform particles and led to lower specific surface area. In contrast, microspheres with larger specific surface area were formed by self-assembly of nanosheets using solvothermal method. ZnFe₂O₄ was the only detectable phase in the fresh C-2Fe-1Zn/K, S-3Fe-1Zn/K and S-2Fe-1Zn/K samples. ZnFe₂O₄ and ZnO co-existed with increasing Zn content in S-1Fe-1Zn/K sample, while ZnO and Fe₂O₃ could be observed over H-2Fe-1Zn/K sample. All the used samples contained Fe3O4, ZnO and Fe₅C₂. The peak intensity of ZnO was strong in the AR-H-2Fe-1Zn/K sample while it was the lowest in the AR-C-2Fe-1Zn/K sample after reaction. The formation of ZnFe₂O₄ increased the interaction between iron and zinc for C-2Fe-1Zn/K and S-Fe-Zn/K samples, causing easier reduction of Fe₂O₃ to Fe3O4. The surface basicity of the sample prepared by co-precipitation method was much more than that of the other two methods. During CO₂ hydrogenation, all the catalysts showed good activity and olefin selectivity. The CO selectivity was increased with increasing Zn content over S-Fe-Zn/K samples. H-2Fe-1Zn/K catalyst preferred to the production of C₅⁺ hydrocarbons. CO₂ conversion of 54.76% and C₂⁼-C₄⁼ contents of 57.38% were obtained on C-2Fe-1Zn/K sample, respectively.

Key words: CO₂ hydrogenation, Light olefins, Preparation methods, Iron-zinc catalyst

Xu Wang, Jianli Zhang, Jingyu Chen, Qingxiang Ma, Subing Fan, Tiansheng Zhao. Effect of preparation methods on the structure and catalytic performance of Fe-Zn/K catalysts for CO₂ hydrogenation to light olefins[J]. Chinese Journal of Chemical Engineering, 2018, 26(4): 761-767.

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Effect of preparation methods on the structure and catalytic performance of Fe-Zn/K catalysts for CO₂ hydrogenation to light olefins

Effect of preparation methods on the structure and catalytic performance of Fe-Zn/K catalysts for CO₂ hydrogenation to light olefins

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