Xu Zhiqiang, Ma Hongfang, Huang Yuxuan, Qian Weixin, Zhang Haitao, Ying Weiyong
State Key Laboratory of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, China.
ACS Omega. 2020 Sep 17;5(38):24574-24583. doi: 10.1021/acsomega.0c03075. eCollection 2020 Sep 29.
Submicron SSZ-13 with different acidities was synthesized successfully with the assistance of nanosized SSZ-13 seeds. The methanol-to-olefins (MTO) properties of submicron SSZ-13 were evaluated. The lifetime of submicron SSZ-13 was enhanced because of the crystal size reduction. The selectivity of light olefins was improved evidently at the early stage of the MTO reaction as the acidity density decreased. TG, GC-MS, and in situ UV/vis spectra were utilized to investigate coking behavior during the MTO reaction. It was found that the acidity density influences the nature and rate of coke formation. The majority of the hydrocarbon pool species over SSZ-13 with a low acidity density (125.2 μmol/g) were methylated benzene carbocations, while that over SSZ-13 with a high acidity density (330.2 μmol/g) were methylated naphthalene carbocations. The low acidity density of SSZ-13 can suppress the hydrogen transfer reaction and polyaromatic generation.
在纳米级SSZ-13晶种的辅助下成功合成了具有不同酸度的亚微米级SSZ-13。对亚微米级SSZ-13的甲醇制烯烃(MTO)性能进行了评估。由于晶体尺寸减小,亚微米级SSZ-13的寿命得以延长。随着酸度密度降低,在MTO反应早期轻质烯烃的选择性明显提高。利用热重分析(TG)、气相色谱-质谱联用(GC-MS)和原位紫外/可见光谱研究了MTO反应过程中的结焦行为。发现酸度密度影响焦炭形成的性质和速率。酸度密度低(125.2 μmol/g)的SSZ-13上的大部分烃池物种是甲基化苯碳正离子,而酸度密度高(330.2 μmol/g)的SSZ-13上的是甲基化萘碳正离子。SSZ-13的低酸度密度可以抑制氢转移反应和多芳烃的生成。