Citation: Ya-Bo SHI, Guo-Qiang ZHANG, Yu-Chen SUN, Hua-Yan ZHENG, Zhong LI, Ju SHANGGUAN, Jie MI, Shou-Jun LIU, Peng-Zheng SHI. KIT-6 Supported CeO₂ for Catalytic Synthesis of Dimethyl Carbonate from CO₂ and Methanol[J]. Chinese Journal of Inorganic Chemistry, ;2021, 37(6): 1004-1016. doi: 10.11862/CJIC.2021.129 shu

KIT-6 Supported CeO₂ for Catalytic Synthesis of Dimethyl Carbonate from CO₂ and Methanol

1.
Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China
2.
College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, China
3.
Taiyuan Green Coke Energy Co., Ltd., Taiyuan 030006, China

Corresponding author: Guo-Qiang ZHANG, zgq198615@163.com Zhong LI, lizhong@tyut.edu.cn
Received Date: 19 December 2020
Revised Date: 10 March 2021

Figures(12)

A series of KIT-6 were synthesized by hydrothermal method at varied aging temperatures (80, 100, 120 and 150℃), which were used as supports to fabricate CeO₂/KIT-6 catalysts. Combined with X-ray diffraction, N₂-physisorption, temperature-programmed desorption of NH₃ and CO₂, transmission electron microscopy, Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy results, the effect of aging temperatures on the structure of KIT-6 and the catalytic activity of CeO₂/KIT-6 for direct synthesis of dimethyl carbonate (DMC) from CO₂ and methanol were investigated in detail. The results indicated that the KIT-6 synthesized at different aging temperatures maintained their unique three-dimensional pore structure. With the increasing aging temperature, the surface areas of KIT-6 firstly increased and then decreased, which attained the maximum (683 m²·g^-1) as the aging temperature was 100℃. High surface areas of KIT-6 favor for the dispersion of CeO₂ and thus improve the number of exposed active sites. The catalytic activity increases with the improved number of the medium base/acid adsorption sites and content of Ce³⁺. Herein, the particle size of CeO₂ for CeO₂/100-KIT-6 was the smallest (5.9 nm) and therefore the number of exposed active sites reached the maximum, which contributed to the optimal catalytic activity. Moreover, the effect of reaction temperature and pressure on the catalytic activity of CeO₂/100-KIT-6 were studied. The results showed that the catalytic activity firstly increased and then decreased with the increasing reaction temperature, and attained the highest as the reaction temperature was 140℃. In addition, the catalytic activity increased with the increase of reaction pressure. Furthermore, the recycle stability of CeO₂/100-KIT-6 was also studied under 140℃ and 6.8 MPa. The results showed that the DMC yield decreased from 15 mmol·g_CeO₂^-1 to 2.8 mmol·g_CeO₂^-1 after recycle six times, which is due to the decrease of active sites resulting from the agglomeration of CeO₂ nanoparticles.
- CO₂,
- CeO₂/KIT-6,
- dimethyl carbonate,
- particle size,
- active sites
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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

KIT-6 Supported CeO2 for Catalytic Synthesis of Dimethyl Carbonate from CO2 and Methanol

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通讯作者: 陈斌, bchen63@163.com

KIT-6 Supported CeO₂ for Catalytic Synthesis of Dimethyl Carbonate from CO₂ and Methanol