Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2018-10-09 , DOI: 10.1016/j.cej.2018.10.053 Mithun Sarker , Nazmul Abedin Khan , Dong Kyu Yoo , Biswa Nath Bhadra , Jong Won Jun , Tae-Wan Kim , Chul-Ung Kim , Sung Hwa Jhung
The conversion of Y zeolites having wide silica/alumina ratio (SAR, 5.1–80) into SSZ-13s was carried out in the presence of N,N,N-dimethylethylcyclohexylammonium (DMCHA) ion, as an organic structure directing agent (OSDA). SSZ-13 zeolites could be obtained from siliceous Y zeolites; however, another phase, analcime (ANA) was obtained when aluminous Y zeolites (SAR: 5.1–12) were converted. Sodium silicate was used not only to successfully convert the aluminous Y zeolites into SSZ-13s but also to increase the SAR of the obtained SSZ-13 zeolites. The synthesis of SSZ-13 with DMCHA was possible in the absence of any seed, which is advantageous in the viewpoint of both the expense and convenience of the synthesis. Moreover, the synthesized SSZ-13s were utilized in the direct conversion of ethylene-to-propylene (ETP). Moderately siliceous SSZ-13s (SAR: 18–24) showed better performance in ETP than aluminous or siliceous SSZ-13s. DMCHA-derived SSZ-13 was also competitive or better in ETP than SSZ-13s prepared with other reported templates including N,N,N-trimethyl-1-adamantanamine hydroxide (TMAda-OH). For example, the maximum propylene yield in ETP over SSZ-13s (with similar SAR of 15–19) prepared with choline chloride, tetraethylammonium hydroxide (TEA-OH), TMAda-OH, and DMCHA-Br were 51, 61, 65 and 68%, respectively. Based on the syntheses and ETP reactions, DMCHA ion can be recommended as a versatile/inexpensive OSDA for the conversion of Y (with wide SARs) into SSZ-13 zeolites which can be effective in ETP reaction. However, further work is required to understand the reason of the competitiveness of the DMCHA-derived SSZ-13 and the effect of the SAR on the propylene yield in ETP.
中文翻译:
在二甲基乙基环己基铵离子存在下合成SSZ-13沸石,并用SSZ-13将乙烯直接转化为丙烯
具有N / N,N-二甲基乙基环己基铵(DMCHA)离子作为有机结构导向剂(OSDA)的情况下,将具有宽二氧化硅/氧化铝比(SAR,5.1–80)的Y沸石转化为SSZ-13s。 。可以从硅质Y型沸石获得SSZ-13型沸石。然而,当铝质Y型沸石(SAR:5.1–12)转化后,便获得了另一种形式的碱金属消解剂(ANA)。硅酸钠不仅用于成功地将铝质Y型沸石转化为SSZ-13s,而且还用于提高所得SSZ-13型沸石的SAR。在没有任何种子的情况下,可以用DMCHA合成SSZ-13,从合成的费用和方便性的角度来看,这是有利的。而且,合成的SSZ-13s被用于乙烯到丙烯(ETP)的直接转化中。中度硅质SSZ-13s(SAR:18–24)在ETP中显示出比铝质或硅质SSZ-13更好的性能。DMCHA衍生的SSZ-13在ETP中也比使用其他报道的模板(包括N,N,N-三甲基-1-金刚烷胺氢氧化物(TMAda-OH))制备的SSZ-13更具竞争力或更好。例如,用氯化胆碱,氢氧化四乙铵(TEA-OH),TMAda-OH和DMCHA-Br制备的SSZ-13s(SAR相似的SAR 19-19)在ETP中的最大丙烯收率是51、61、65和分别为68%。基于合成和ETP反应,可以推荐DMCHA离子作为通用/廉价的OSDA,用于将Y(具有宽SAR)转化为可在ETP反应中有效的SSZ-13沸石。但是,需要做进一步的工作来理解DMCHA衍生的SSZ-13的竞争力的原因以及SAR对ETP中丙烯收率的影响。