Study on the catalytic performance of fe <i>in situ</i> modified small crystallite silicalite-1 zeolite in chichibabin condensation reaction

TAO Jinquan; JIA Yijing; BAI Tianyu; HUANG Wenbin; CUI Yan; ZHOU Yasong; WEI Qiang

doi:10.1016/S1872-5813(24)60443-3

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TAO Jinquan, JIA Yijing, BAI Tianyu, HUANG Wenbin, CUI Yan, ZHOU Yasong, WEI Qiang. Study on the catalytic performance of fe in situ modified small crystallite silicalite-1 zeolite in chichibabin condensation reaction[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(24)60443-3

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TAO Jinquan, JIA Yijing, BAI Tianyu, HUANG Wenbin, CUI Yan, ZHOU Yasong, WEI Qiang. Study on the catalytic performance of fe in situ modified small crystallite silicalite-1 zeolite in chichibabin condensation reaction[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(24)60443-3

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Study on the catalytic performance of fe in situ modified small crystallite silicalite-1 zeolite in chichibabin condensation reaction

doi: 10.1016/S1872-5813(24)60443-3

TAO Jinquan^{1, 2
,},
JIA Yijing^1
,,
BAI Tianyu^1
,,
HUANG Wenbin^1
,,
CUI Yan^2
,,
ZHOU Yasong^1
,,
WEI Qiang^{1
,
,}

1.
China University of Petroleum-Beijing, Beijing 102206, China
2.
PetroChina Petrochemical Research Institue, Beijing 102206, China

Received Date: 2024-02-27
Accepted Date: 2024-03-20
Rev Recd Date: 2024-03-20

Available Online: 2024-04-10

Abstract

Abstract

Pyridine and its derivatives, collectively referred to as pyridine bases, find extensive applications in fields such as pesticides and pharmaceuticals, serving as crucial intermediates in the chemical industry. In recent years, with the development of the pesticide and pharmaceutical industries, the demand for pyridine bases has rapidly increased. The Chichibabin condensation reaction is the most widely used route for industrial production of pyridine bases. Currently, the most commonly used ZSM-5 zeolite catalyst is limited by the instability of its silicon-aluminum framework structure, resulting in a short active reaction cycle (5 hours). In response to this issue, this study selected the thermally stable and hydrothermally stable Silicalite-1 zeolite. Polyvinylpyrrolidone (PVP) was employed as a colloidal dispersant using a hydrothermal synthesis method. In situ modification was utilized to introduce Fe into the MFI framework during zeolite synthesis. The influence of PVP dosage, template agent dosage, and other crystallization conditions on the crystallinity, pore structure, and acidity of Silicalite-1 zeolite products was investigated using X-ray diffraction (XRD), scanning electron microscopy (SEM), thermogravimetric analysis (TG), and BET surface area analysis. The acidity of Fe-modified Silicalite-1 zeolites was characterized using NH₃-temperature programmed desorption (NH₃-TPD), pyridine infrared (Py-FTIR) spectroscopy, Fourier-transform infrared (FT-IR) spectroscopy, and X-ray photoelectron spectroscopy (XPS). Experimental results indicated that the addition of seed crystals effectively reduced the particle size of the molecular sieve to approximately 200 nm. Fe-modified Silicalite-1 exhibited a disk-like morphology with good crystal dispersion. The highest relative crystallinity of the product reached 103% with a seed crystal input of 15% and PVP addition of 3.75%. Fe-modified Silicalite-1 possessed a greater abundance of both Lewis (L) and Brønsted (B) acid sites. The modified Silicalite-1 exhibits a higher abundance of B and L acid sites, resulting in an increase in the initial activity for the pyridine bases synthesis with Chichibabin condensation from 66% to 85%. Compared to ZSM-5, Fe-modified Silicalite-1 exhibited superior catalytic stability, maintaining the conversion rates and yields of pyridine bases above 66% and 40%, respectively, over a 15 hour reaction period. Finally, the strategy proposed in this study, which utilizes polyvinylpyrrolidone as a colloidal stabilizer to modify Silicalite-1 zeolite, significantly broadened the application prospects of weakly acidic pure silica zeolites in the field of acid catalysis. This approach has demonstrated significant scientific value and industrial potential.
- Silicalite-1 zeolites,
- in-situ modification method,
- hydrothermal method,
- catalyst,
- Chichibabin condensation reaction

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References(23)

References

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