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Fluoride-free Synthesis of Mesoporous [Al]-[B]-ZSM-5 using Cetyltrimethylammonium Bromide and Methanol-to-Olefin Activity with High Propene Selectivity
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2020-11-05 , DOI: 10.1016/j.apcata.2020.117915
Busra Karakaya Yalcin , Bahar Ipek

Large ZSM-5 crystals containing [B]-sites and mesopores with 2.5 nm pore sizes are synthesized in a fluoride-free low OH- medium using cethyltrimethylammonium bromide as mesoporogen and 1,6-diaminohexane as structure directing agent. Absence of extra-framework Al sites and low concentrations of silanol sites are evidenced by 27Al MAS-NMR and in-situ FTIR analysis. The low-defect containing [Al]-[B]-ZSM-5 (Mes-[Al]-[B]-ZSM-5) is evaluated for catalyzing the methanol-to-olefins reaction and found to result in low coke formation (4.1 mg g-1 h-1) and very low alkane and aromatic formation rates. The propene to ethene ratio of 4.3 observed using Mes-[Al]-[B]-ZSM-5 is found to be superior to that (1.9) of a nano-sized [Al]-[B]-ZSM-5 (crystal sizes around 36 nm). Small particle sizes for nano-sized [Al]-[B]-ZSM-5 is found to be effective for supplying a higher coke tolerance, but insignificant for olefin product selectivity.



中文翻译:

十六烷基三甲基溴化铵和甲醇制烯烃的高丙烯选择性无氟合成介孔[Al]-[B] -ZSM-5

使用溴化乙基三甲基铵作为介孔原和1,6-二氨基己烷作为结构导向剂,在无氟化物的低OH-介质中合成了具有[B]位和孔径为2.5 nm的中孔的大型ZSM-5晶体。27 Al MAS-NMR和原位FTIR分析证明没有骨架外的Al位点和低浓度的硅烷醇位点。对低缺陷的[Al]-[B] -ZSM-5(Mes- [Al]-[B] -ZSM-5)进行了催化甲醇制烯烃反应的评估,结果发现生成的焦炭少(4.1毫克g -1  h -1)和非常低的烷烃和芳烃生成速率。发现使用Mes- [Al]-[B] -ZSM-5观察到的丙烯与乙烯之比为4.3,优于纳米级[Al]-[B] -ZSM-5(晶体)的(1.9)。尺寸约36 nm)。发现纳米尺寸[Al]-[B] -ZSM-5的小粒径可有效提供更高的焦炭耐受性,但对烯烃产物的选择性却微不足道。

更新日期:2020-11-06
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