Citation: ZHAI Yanliang, ZHANG Shaolong, ZHANG Luoming, SHANG Yunshan, WANG Wenxuan, SONG Yu, JIANG Caitong, GONG Yanjun. Effect of B and Al Distribution in ZSM-5 Zeolite on Methanol to Propylene Reaction Performance[J]. Acta Physico-Chimica Sinica, ;2019, 35(11): 1248-1258. doi: 10.3866/PKU.WHXB201901062 shu

Effect of B and Al Distribution in ZSM-5 Zeolite on Methanol to Propylene Reaction Performance

State Key Laboratory of Heavy Oil Processing, the Key Laboratory of Catalysis of CNPC, College of Chemistry Engineering and Environment, China University of Petroleum, Beijing 102249, P. R. China

Corresponding author: GONG Yanjun, gongyj@cup.edu.cn
Received Date: 24 January 2019
Revised Date: 20 February 2019
Accepted Date: 4 March 2019
Available Online: 8 November 2019
Fund Project: The project was supported by the National Natural Science Foundation of China (U1662116, 21276278)the National Natural Science Foundation of China U1662116the National Natural Science Foundation of China 21276278

Propylene is widely used as a raw material for producing polypropylene, acrylonitrile, propylene oxide, etc. Typical manufacturing processes for propylene (steam cracking and FCC process) are over-reliant on petroleum resources and cannot meet the rapidly growing global demands. New routes for producing propylene from non-oil resources, particularly methanol-to-propylene (MTP) technology, have attracted increasingly more attention, where a fixed-bed reactor is used and ZSM-5 zeolite is the best alternative catalyst. However, structural optimization of ZSM-5 to enhance the lifetime and propylene selectivity and a deep understanding of the mechanism of the MTP reaction are still considerable challenges. For the conventional ZSM-5 zeolite, carbon deposition preferentially occurs near the outer surface of the zeolite particles because of the high acid density on the external surface, which accelerates the deactivation by blocking the outer pore openings, especially in a long-term MTP reaction. Large amounts of external strong acids also promote secondary reactions, such as hydrogen transfer reactions, resulting in a decrease in propylene selectivity. To study the effects of strong and weak acid distributions of ZSM-5 zeolite on the MTP reaction, two series of boron-modified ZSM-5 zeolites were designed: B-Al-ZSM-5 zeolites by one-step synthesis and Al-ZSM-5@B-ZSM-5 core-shell zeolites by two-step synthesis. These were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), scanning transmission electron microscopy (STEM) mapping, N₂ physical adsorption-desorption, temperature-programmed desorption of ammonia (NH₃-TPD) and 1, 3, 5-triisopropylbenzene (TIPB) cracking, and B1-Al-ZSM-5 and Al@B1-ZSM-5, B2-Al-ZSM-5 and Al@B2-ZSM-5, and B3-Al-ZSM-5 and Al@B3-ZSM-5 samples in the two series were found to have similar texture properties, acid amounts and acid strengths, but different B and Al elemental distributions and acid distributions. We used these two sets of samples to compare the effect of different strong and weak acid distributions—a uniform distribution and a gradient distribution of strong and weak acids on the performance of the MTP reaction. The results showed that samples with a uniform distribution of strong and weak acids have higher propylene selectivity due to lower strong and weak acid densities, whereas samples with a gradient acid distribution have a longer catalytic lifetime in the MTP reaction due to the absence of strong acid density and higher weak acid density on the outer surface. The different acid distributions lead to two different carbon deposition modes. Carbon deposition of the sample with the uniform acid distribution preferentially formed on the outer surface, resulting in rapid deactivation by blocking external micropores and leaving the internal active centers not fully utilized. However, for the sample with the gradient acid distribution, the carbon-blocking rate of the external surface considerably decreased, which increased the time that the reactant molecules had to enter the internal micropores. Thus, the utilization rate of the active centers and the catalytic lifetime of the Al-ZSM-5@B-ZSM-5 core-shell sample considerably increased.
- B-Al-ZSM-5,
- Al-ZSM-5@B-ZSM-5,
- Core-shell zeolite,
- Acid distribution,
- Methanol to propylene
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