ABSTRACT
During prior investigations of the synthesis of the novel zeolite YNU-5 (YFI), it was found that a very slight amount of an impurity phase contaminated the desired zeolitic phase. This impurity was very often ZSM-5 (MFI). The phase composition was determined to be sensitive to the water in the synthesis mixture, and it was possible to obtain a pure phase and also to intentionally generate a specific impurity phase. In the present work, trials based on the dimethyl ether-to-olefin (DTO) reaction using a fixed-bed downflow reactor were performed to assess the effect of the purity of YNU-5 on its catalytic performance. Dealuminated pure YNU-5 exhibited rapid deactivation due to coking at time on stream (TOS) values exceeding 5 min. Surprisingly, this deactivation was greatly suppressed when the material contained a trace amount of ZSM-5 consisting of nano-sized particles. The formation of ZSM-5 nanoparticles evidently improved the performance of the catalytic system during the DTO reaction. The product distributions obtained from this reaction using highly dealuminated and very pure YNU-5 resembled those generated by 12-ring rather than 8-ring zeolite catalysts. The high selectivity for desirable C3 and C4 olefins during the DTO reaction over YNU-5 is beneficial.
ABSTRACT
Synthesis of new zeolites with controlled pore architectures is important in the field of catalysis and separation related to chemical transformation, environmental protection, and energy-saving. Zeolites containing channels of different sizes in the same framework have been desirable. We report here the synthesis and structure of a novel aluminosilicate zeolite (designated as YNU-5), the first zeolite containing interconnected 12-, 12-, and 8-ring pores, as well as independent straight 8-ring channels. The synthesis procedure is quite simple and consists of conventional hydrothermal conditions as well as readily available starting materials. The framework structure is stable enough and Si/Al ratio is controllable between 9 and 350. Determination of the crystal structure is performed by utilizing X-ray diffraction-based techniques, revealing 9 independent tetrahedrally coordinated atoms. This robust structure is expected to be industrially valuable and several unusual combinations of composite building units are of considerable interest in an academic sense. The new zeolite YNU-5 is promising catalyst for the production of useful light olefins such as propylene and butylenes in the dimethyl ether-to-olefin reaction, when the Si/Al ratio is properly tuned by dealumination through simple acid treatments.
