Citation: Bao-Lian ZHANG, Chang LIU, Su LIU, Hai-Bo ZHOU, Jun-Jie SU, Yang-Dong WANG, Dong-Sen MAO. ZnCr₂O₄/ZSM-5@Silicalite-1 to optimize the selectivity of one-step hydrogenation of CO₂ to aromatics[J]. Chinese Journal of Inorganic Chemistry, ;2023, 39(12): 2339-2348. doi: 10.11862/CJIC.2023.195 shu

ZnCr₂O₄/ZSM-5@Silicalite-1 to optimize the selectivity of one-step hydrogenation of CO₂ to aromatics

Bao-Lian ZHANG ^{1, 2} ,
Chang LIU ² ,
Su LIU ² ,
Hai-Bo ZHOU ² ,
Jun-Jie SU ² ,
Yang-Dong WANG ^2,, ,
Dong-Sen MAO ^1,,

1.
School of Chemical and Environment Engineering, Shanghai Institute of Technology, Shanghai 201418, China
2.
State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Sinopec Shanghai Research Institute of Petrochemical Technology Co., Ltd., Shanghai 201208, China

Corresponding author: Yang-Dong WANG, wangyd.sshy@sinopec.com Dong-Sen MAO, dsmao@sit.edu.cn
Received Date: 13 April 2023
Revised Date: 2 November 2023

Figures(9)

The CO₂ hydrogenation reaction over the oxide-zeolite bifunctional catalyst yields a mixture of BTX (benzene, toluene, and xylene), C₉, and C₁₀₊ aromatic products, among which BTX is of the highest commercial value. To improve the distribution of the aromatic products and promote the production of BTX, the core-shell structured zeolite ZSM-5@Silicalite-1 was prepared by the epitaxial growth method in this work. According to the characterization results of powder X-ray diffraction (PXRD), N₂ adsorption-desorption, temperature-programmed desorption of NH₃ (NH₃-TPD), scanning electron microscope (SEM), transmission electron microscopy (TEM), and pyridine adsorption Fourier transform infrared spectroscopy (Py-IR), the inert Silicalite-1 shell is uniformly coated on the external surface of the ZSM-5 core, therefore changes its acidic properties especially reduces the external acidity, which contributes to improving the aromatic distribution. When applied in the one-step CO₂-to-aromatic reaction, the combination of ZSM-5@Silicalite-1 and Zn-Cr oxide resulted in a CO₂ conversion of 21.9% and aromatics selectivity of 79.3% under the conditions of V_H₂/V_CO₂=3.0, 1 200 mL·g^-1·h^-1, 320 ℃, and 4.0 MPa, and it gave a 33.5% of light aromatics in the overall aromatics, which was higher than 14.8% over the ZnCr₂O₄/ZSM-5 system. Additionally, in the one-step CO₂-to-aromatic reaction system, the by-products of CO and H₂O are generated from the side reaction of reverse water-gas shift (RWGS). Due to the higher hydrophobicity of Silicalite-1 than ZSM-5, H₂O is enriched at the interface between the oxide and core-shell zeolite, which can shift the reaction equilibrium of RWGS, thus inhibiting the generation of CO. As a result, the CO selectivity was significantly reduced at high space velocities compared with the unmodified oxide-zeolite system. At an optimal shell thickness, the ZnCr₂O₄/ZSM-5@Silicalite-1 bifunctional catalyst obtained a space-time yield of aromatics of 2.4 mmol·g^-1·h^-1 at 8 400 mL·g^-1·h^-1, which was 22% higher compared with ZnCr₂O₄/ZSM-5.
- carbon dioxide,
- aromatics,
- bifunctional catalysis,
- reaction path,
- core-shell zeolite
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ZnCr₂O₄/ZSM-5@Silicalite-1 to optimize the selectivity of one-step hydrogenation of CO₂ to aromatics