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

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

Pengfei Wu ^a,b, ,
Miao Yang ^a ,
Wenna Zhang ^a,b ,
Shu Zeng ^a,b ,
Mingbin Gao ^a,b ,
Shutao Xu ^a ,
Peng Tian ^a ,
Zhongmin Liu ^a

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 100049, China

Received Date: 7 May 2018
Revised Date: 2 June 2018

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

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.
- N,N'-dimethylethylenediamine,
- SAPO molecular sieves,
- Synthesis,
- DNL-6,
- Methanol amination reaction
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