Influence of Zr, Ce, and La on Co3O4 catalyst for CO2 methanation at low temperature

doi:10.1016/j.cjche.2017.10.014

Chin.J.Chem.Eng. ›› 2018, Vol. 26 ›› Issue (4): 768-774.DOI: 10.1016/j.cjche.2017.10.014

• Catalysis, Kinetics and Reaction Engineering • Previous Articles Next Articles

Influence of Zr, Ce, and La on Co₃O₄ catalyst for CO₂ methanation at low temperature

Yuwen Zhou¹, Yuexiu Jiang¹, Zuzeng Qin^1,2, Qinruo Xie³, Hongbing Ji^1,2

1 School of Chemistry and Chemical Engineering, Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology, Guangxi University, Nanning 530004, China;
2 School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China;
3 School of Biology and Chemical Engineering, Guangxi University of Science and Technology, Liuzhou 545006, China

Received:2017-07-30 Revised:2017-07-30 Online:2018-05-19 Published:2018-04-28
Contact: Zuzeng Qin,E-mail addresses:qinzuzeng@gmail.com,qinzuzeng@gxu.edu.cn;Hongbing Ji,E-mail addresses:jihb@mail.sysu.edu.cn
Supported by:
Supported by the National Natural Science Foundation of China (21366004), Guangxi Natural Science Foundation (2016GXNSFFA380015), the Dean Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology (2016Z003).

Influence of Zr, Ce, and La on Co₃O₄ catalyst for CO₂ methanation at low temperature

Yuwen Zhou¹, Yuexiu Jiang¹, Zuzeng Qin^1,2, Qinruo Xie³, Hongbing Ji^1,2

1 School of Chemistry and Chemical Engineering, Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology, Guangxi University, Nanning 530004, China;
2 School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China;
3 School of Biology and Chemical Engineering, Guangxi University of Science and Technology, Liuzhou 545006, China

通讯作者: Zuzeng Qin,E-mail addresses:qinzuzeng@gmail.com,qinzuzeng@gxu.edu.cn;Hongbing Ji,E-mail addresses:jihb@mail.sysu.edu.cn
基金资助:
Supported by the National Natural Science Foundation of China (21366004), Guangxi Natural Science Foundation (2016GXNSFFA380015), the Dean Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology (2016Z003).

Abstract

Abstract: The Co₃O₄ and Zr-, Ce-, and La-Co₃O₄catalysts were prepared, characterized, and applied to produce CH₄ from CO₂ catalytic hydrogenation in low temperature as 140-220℃. The results indicated that the addition of Zr, Ce, or La to the Co₃O₄ decreased the crystallite sizes of Co and the outer-shell electron density of Co³⁺, and increased the specific surface area, which would provide more active sites for the CO₂ methanation. Especially, the addition of Zr also changed the reducing state of Co₃O₄ via an obvious change in the interaction between Co₃O₄ and ZrO₂. Furthermore, Zr doped into the Co₃O₄ increased the basic intensity of the weak and medium basic sites, as well as the amount of Lewis acid sites, and Brønsted acid sites were also found on the Zr-Co₃O₄ surface. The introduction of Zr, Ce, or La favored the production of CH₄, and the Zr-Co₃O₄ catalyst exhibited the highest CO₂ conversion (58.2%) and CH₄ selectivity (100%) at 200℃, and 0.5 MPa with a gaseous hourly space velocity of 18,000 ml·g_cat^-1·h^-1, and the catalytic activity of CO₂ methanation for the Zr-, Ce-, and La-Co₃O₄ exhibited more stable than Co₃O₄ in a 20-h reaction.

Key words: CO₂ hydrogenation, Methanation, Co₃O₄ catalyst, Cobalt-zirconium interaction, Basic sites

摘要： The Co₃O₄ and Zr-, Ce-, and La-Co₃O₄catalysts were prepared, characterized, and applied to produce CH₄ from CO₂ catalytic hydrogenation in low temperature as 140-220℃. The results indicated that the addition of Zr, Ce, or La to the Co₃O₄ decreased the crystallite sizes of Co and the outer-shell electron density of Co³⁺, and increased the specific surface area, which would provide more active sites for the CO₂ methanation. Especially, the addition of Zr also changed the reducing state of Co₃O₄ via an obvious change in the interaction between Co₃O₄ and ZrO₂. Furthermore, Zr doped into the Co₃O₄ increased the basic intensity of the weak and medium basic sites, as well as the amount of Lewis acid sites, and Brønsted acid sites were also found on the Zr-Co₃O₄ surface. The introduction of Zr, Ce, or La favored the production of CH₄, and the Zr-Co₃O₄ catalyst exhibited the highest CO₂ conversion (58.2%) and CH₄ selectivity (100%) at 200℃, and 0.5 MPa with a gaseous hourly space velocity of 18,000 ml·g_cat^-1·h^-1, and the catalytic activity of CO₂ methanation for the Zr-, Ce-, and La-Co₃O₄ exhibited more stable than Co₃O₄ in a 20-h reaction.

关键词: CO₂ hydrogenation, Methanation, Co₃O₄ catalyst, Cobalt-zirconium interaction, Basic sites

Yuwen Zhou, Yuexiu Jiang, Zuzeng Qin, Qinruo Xie, Hongbing Ji. Influence of Zr, Ce, and La on Co₃O₄ catalyst for CO₂ methanation at low temperature[J]. Chin.J.Chem.Eng., 2018, 26(4): 768-774.

Yuwen Zhou, Yuexiu Jiang, Zuzeng Qin, Qinruo Xie, Hongbing Ji. Influence of Zr, Ce, and La on Co₃O₄ catalyst for CO₂ methanation at low temperature[J]. Chinese Journal of Chemical Engineering, 2018, 26(4): 768-774.

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Influence of Zr, Ce, and La on Co₃O₄ catalyst for CO₂ methanation at low temperature

Influence of Zr, Ce, and La on Co₃O₄ catalyst for CO₂ methanation at low temperature

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