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One-pot green synthesis of Fe-ZSM-5 zeolite containing framework heteroatoms via dry gel conversion for enhanced propylene selectivity of catalytic cracking catalyst

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Abstract

Development of a sustainable route for the synthesis of Fe-ZSM-5 zeolites is important due to their diverse applications in different fields. Herein, we report a novel, efficient and an eco-friendly dry gel conversion method to one-pot synthesize Fe-ZSM-5 zeolite containing framework heteroatoms under the conditions that neither the template nor the seed crystal was added. The present strategy not only improves the synthesis efficiency of zeolites, but also reduces the cost and environmental pollution by avoiding using ordinary template. The physicochemical properties of the synthesized samples were analyzed by XRD, N2 adsorption–desorption, SEM, UV–visible diffuse reflectance, XPS, FT-IR and NH3-TPD techniques. The characterization results revealed that the Fe species in the one-pot synthesized Fe-ZSM-5 zeolite (Fe-ZSM-5-In) mainly exist in the zeolite framework in the form of Fe3+, while those in the Fe/ZSM-5 zeolite prepared by impregnation (Fe/ZSM-5-Im) mostly exist on the surface of the zeolite in the form of non-framework Fe such as oligomeric Fex3+Oy clusters and Fe2O3 particles. Fe-ZSM-5-In possessed enhanced acid amount and better distribution of framework Fe3+ species than Fe/ZSM-5-Im. The results of catalytic performance evaluation show that the propylene yield is improved by the Fe modified ZSM-5 additives due to enhanced acid content and acid strength. Compared with the Fe/ZSM-5-Im additive, the Fe-ZSM-5-In additive has higher propylene yield and lower coke yield owing to its more acid content and lower dehydrogenation activity.

Graphical Abstract

The Fe-ZSM-5 zeolite containing the framework heteroatoms was one-pot synthesized by the dry gel conversion (DGC) method under the conditions that neither the template nor the seed crystal is added, which exhibits improv ed catalytic activity and has higher propylene yield than the Fe/ZSM-5 additive in the catalytic cracking process.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (21776311 and 21908240), Shandong Provincial Natural Science Foundation, China (ZR2016BM28), National Key Technologies R & D Program of China, Key Projects of Intergovernmental International Innovation Cooperation (2018YFE0118200), Key Research and Development Project of Shandong Province (2019JZZY010506) and National Training Program of Innovation and Entrepreneurship for Undergraduates (20190115).

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Authors and Affiliations

  1. State Key Laboratory of Heavy Oil Processing, College of Science, China University of Petroleum (East China), Qingdao, 266580, China

    Youhe Wang, Tingting Li, Chencan Li, Jinzhi Lu, Chang Dai, Fazle Subhan, Peng Bai, Hongman Sun & Zifeng Yan

  2. Shandong High-End Chemical Research Institute, Heze, Shandong, 274002, China

    Chencan Li

  3. Department of Chemistry, Abdul Wali Khan University Mardan, Mardan, KP , Pakistan

    Fazle Subhan

  4. School of Chemical Engineering & Technology, China University of Mining & Technology, Xuzhou, Jiangsu, 221116, China

    Rui Feng

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  1. Youhe Wang
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Wang, Y., Li, T., Li, C. et al. One-pot green synthesis of Fe-ZSM-5 zeolite containing framework heteroatoms via dry gel conversion for enhanced propylene selectivity of catalytic cracking catalyst. J Mater Sci 56, 18050–18060 (2021). https://doi.org/10.1007/s10853-021-06472-2

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