Silicoaluminophosphate molecular sieve DNL-6: Synthesis with a novel template, N,N'-dimethylethylenediamine, and its catalytic application

doi:10.1016/S1872-2067(18)63122-5

Abstract

Abstract:

DNL-6, a silicoaluminophosphate (SAPO) molecular sieve with RHO topology, was hydrothermally synthesized using a new structure-directing agent (SDA), N,N'-dimethylethylenediamine. The obtained samples were characterized by X-ray diffraction, X-ray fluorescence, X-ray photoelectron spectroscopy, scanning electron microscopy, and N₂ adsorption, which indicated that the synthesized DNL-6s have high crystallinity and relatively high Si content ranging from 20% to 35%. Solid-state magic-angle-spinning (MAS) nuclear magnetic resonance (¹³C, ²⁹Si, ²⁷Al, ³¹P, and ²⁷Al multiple-quantum (MQ)) was conducted to investigate the status of the SDA and local atomic environment in the as-synthesized DNL-6. Thermal analysis revealed the presence of a large amount of amines in the DNL-6 crystals (about 4.4 SDAs per α-cage), which was the reason for the formation of DNL-6 with an ultrahigh Si content (36.4% Si per mole). Interestingly, DNL-6 exhibited excellent catalytic performance for methanol amination. More than 88% methanol conversion and 85% methylamine plus dimethylamine selectivity could be achieved due to the combined contribution of strong acid sites, suitable acid distribution, and narrow pore dimensions of DNL-6.

Key words: N,N'-dimethylethylenediamine, SAPO molecular sieves, Synthesis, DNL-6, Methanol amination reaction

Pengfei Wu, Miao Yang, Wenna Zhang, Shu Zeng, Mingbin Gao, Shutao Xu, Peng Tian, Zhongmin Liu. Silicoaluminophosphate molecular sieve DNL-6: Synthesis with a novel template, N,N'-dimethylethylenediamine, and its catalytic application[J]. Chinese Journal of Catalysis, 2018, 39(9): 1511-1519.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(18)63122-5

https://www.cjcatal.com/EN/Y2018/V39/I9/1511

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