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Chemical Papers

, Volume 73, Issue 1, pp 221–237 | Cite as

Fast synthesis of hierarchical CHA/AEI intergrowth zeolite with ammonium salts as mineralizing agent and its application for MTO process

  • Na Chang
  • Lu Bai
  • Yanfeng ZhangEmail author
  • Gaofeng ZengEmail author
Original Paper
  • 90 Downloads

Abstract

Fast solvent-free synthesis of hierarchical SAPO-34/18 zeolite was realized by combining oil-bath heating and the addition of catalytic amount of ammonium salt. The obtained zeolite samples were systematically characterized by XRD, SEM, XRF, BET, NH3-TPD, and NMR. XRD and SEM results showed that high-quality SAPO-34/18 nano-crystals with plate morphology can be obtained in only 60 min. The addition of ammonium salt served as mineralizing agent which speeded up the crystallization process in solvent-free precursor. The fast heat transfer of oil-bath heating and seeding also contributed to the ultrafast synthesis. Nitrogen adsorption–desorption analysis indicated the presence of high BET surface area and micropore volume, as well as abundant mesopores and macropores. NH3-TPD and 29Si NMR results showed that the samples exhibited appropriate acid strength and concentration. The obtained SAPO catalysts showed excellent performance in MTO reaction with significantly longer catalytic lifetime and higher propylene and butylene selectivities, compared with micron-sized SAPO-34 catalyst made with the conventional hydrothermal method. The extended lifetime could be attributed to the thin-plate crystal morphology and hierarchical pore structure, which greatly alleviated the diffusion constrain and coke deposition in MTO reaction. Higher propylene and butylene selectivities could be ascribed to the larger size of the AEI cage, which allows the easy diffusion of longer alkenes. The realization of ultrafast synthesis with solvent-free precursor not only reduces the waste disposal and energy consumption, but also increases the autoclave efficiency significantly.

Keywords

Zeolite synthesis SAPO-34 SAPO-18 Solvent-free Oil-bath heating Methanol-to-olefins 

Notes

Acknowledgements

The authors acknowledge the financial support from National 863 Project (No. 2012AA050104), Advanced Coal Project (No. XDA07040400), Zhihong Scholar Project from Shanghai University of Engineering Science and SUES Sino-foreign cooperative innovation center for city soil ecological technology integration (2017PT03).

Supplementary material

11696_2018_574_MOESM1_ESM.docx (14.2 mb)
Supplementary material 1 (DOCX 14538 kb)

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Copyright information

© Institute of Chemistry, Slovak Academy of Sciences 2018

Authors and Affiliations

  1. 1.School of Environmental and Chemical EngineeringShanghai UniversityShanghaiChina
  2. 2.CAS Key Laboratory of Low-carbon Conversion Science and Engineering, Shanghai Advanced Research InstituteChinese Academy of SciencesShanghaiChina
  3. 3.Institute of Condensed Matter and Nanosciences (IMCN), Bio and Soft Matter (BSMA)Université catholique de LouvainLouvain-la-NeuveBelgium
  4. 4.School of Chemistry and Chemical EngineeringShanghai University of Engineering ScienceShanghaiChina

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