Catalysis Communications ( IF 3.4 ) Pub Date : 2023-06-16 , DOI: 10.1016/j.catcom.2023.106718 Ali Al-Shathr , Bashir Y. Al-Zaidi , Amal K. Shehab , Zaidoon M. Shakoor , Safa Aal-Kaeb , Laura Quintana Gomez , Hasan Sh. Majdi , Emad N. Al-Shafei , Adnan A. AbdulRazak , James McGregor
Coke formation inside heterogeneous reactors is an important industrial problem that leads to reduced catalyst efficiency. However, this study aims to prove the benefits of coke build-up in improving catalyst performance. The formation and decomposition of coke on six different zeolite structures was studied. The dissociation kinetic model of the spent catalysts during the toluene alkylation with 1-heptene inside a stainless-steel autoclave reactor at different temperatures was carried out. Various techniques (XRD, XRF, TPO, CHNS and TGA-DTG) were used. It was found that the conversion and selectivity of the desired product were higher on the parent H-mordenite and the dealuminated H-beta catalysts with conversions of 85.3% and 84.67%, respectively, at a 360 min reaction time. This was attributed to the reduction of the ratio of hard:soft coke. It is confirmed that the decomposition activation energies of hard coke, 140.1–202.6 kJ/mol, are much higher energies than those of soft coke, 89.9–118.7 kJ/mol. It is also noted that the hypothesis of pore mouth catalysis is dominated by non-polyaromatic coke on the surface of the H-beta catalysts, while the hypothesis is dominated by polyaromatic coke on the surface of the H-mordenite catalysts.
中文翻译:
根据孔口催化假说,对焦炭积累相对于 Beta 和丝光沸石催化剂的优势进行实验和动力学研究
非均相反应器内的焦炭形成是一个重要的工业问题,会导致催化剂效率降低。然而,这项研究旨在证明焦炭堆积在提高催化剂性能方面的好处。研究了焦炭在六种不同沸石结构上的形成和分解。建立了不锈钢高压釜反应器内不同温度下甲苯与1-庚烯烷基化过程中废催化剂的离解动力学模型。使用了各种技术(XRD、XRF、TPO、CHNS 和 TGA-DTG)。结果发现,母体 H-丝光沸石和脱铝 H-β 催化剂上所需产物的转化率和选择性较高,在 360 分钟的反应时间内,转化率分别为 85.3% 和 84.67%。这是由于硬焦与软焦的比例降低所致。经证实,硬焦的分解活化能为140.1~202.6 kJ/mol,远高于软焦的分解活化能89.9~118.7 kJ/mol。还值得注意的是,孔口催化假说以H-β催化剂表面的非聚芳焦为主,而该假说以H-丝光沸石催化剂表面的聚芳焦为主。