Chinese Journal of Catalysis

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SAPO-34 synthesized with n-butylamine as a template and its catalytic application in the methanol amination reaction

Yuyan Qiaoa,b, Pengfei Wua,b, Xiao Xianga,b, Miao Yanga, Quanyi Wanga, Peng Tiana, Zhongmin Liua   

  1. a National Engineering Laboratory for Methanol to Olefins, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
    b University of Chinese Academy of Sciences, Beijing 100039, China
  • Received:2016-11-28 Revised:2016-12-25 Online:2017-03-18 Published:2017-03-22
  • Supported by:

    This work was supported by the National Natural Science Foundation of China(21676262, 21476228, 21506207) and the Key Research Program of Frontier Sciences of CAS (QYZDB-SSW-JSC040).

Abstract:

SAPO-34 was synthesized with n-butylamine (BA) as a template for the first time. Crystallization temperature and initial Si amount were important factors leading to successful syntheses. Lamellar AlPO-kanemite tends to form as the major phase or as an impurity of SAPO-34 at lower crystallization temperatures, though a higher initial Si amount may offer a positive effect on the crystallization of SAPO-34 that mitigates the low temperature. Higher temperature (240℃) can effectively suppress the generation of lamellar materials and allow the synthesis of pure SAPO-34 with a wider range of Si incorporation. The crystallization processes at 200 and 240℃ were investigated and compared. We used the aminothermal method to synthesize SAPO-34-BA at 240℃ and also found n-propylamine is a suitable template for the synthesis of SAPO-34. The SAPO-34-BA products were characterized by many techniques. SAPO-34-BA has good thermal stability, crystallinity and porosity. BA remained intact in the crystals with ~1.8 BA molecule per chabazite cage. The catalytic performance of SAPO-34 was tested in the methanol amination reaction, which showed high methanol conversion and selectivity for methylamine plus dimethylamine under the conditions investigated, suggesting that this material is a good candidate for the synthesis of methylamines.

Key words: SAPO-34 molecular sieve, n-Butylamine, Primary amine, Synthesis, High temperature, Methanol amination