Frontiers of Chemical Science and Engineering ( IF 4.3 ) Pub Date : 2023-06-12 , DOI: 10.1007/s11705-023-2325-9 Xiangxiang Ren , Zhong-Pan Hu , Jingfeng Han , Yingxu Wei , Zhongmin Liu
Improving the aromatic selectivity in the alkane aromatization process is of great importance for its practical utilization but challenge to make because the high H/C ratio of alkanes would lead to a serious hydrogen transfer process and a large amount of light alkanes. Herein, CO2 is introduced into the cyclohexane conversion process on the HZSM-5 zeolite, which can improve the aromatic selectivity. By optimizing the reaction conditions, an improved aromatic (benzene, toluene, xylene, and C9+) selectivity of 48.2% can be obtained at the conditions of 2.7 MPa (CO2), 450 °C, and 1.7 h−1, which is better than that without CO2 (aromatic selectivity = 43.2%). In situ transmission Fourier transform infrared spectroscopy spectra illustrate that many oxygenated chemical intermediates (e.g., carboxylic acid, anhydride, unsaturated aldehydes/ketones or ketene) would be formed during the cyclohexane conversion process in the presence of CO2. 13C isotope labeling experimental results demonstrate that CO2 can enter into the aromatics through the formation of oxygenated chemical intermediates and thereby improve the aromatic selectivity. This study may open a green, economic, and promising way to improve the aromatic selectivity for alkane aromatization process.
中文翻译:
CO2偶联提高环己烷芳构化的芳烃选择性
提高烷烃芳构化过程中的芳烃选择性对其实际应用具有重要意义,但由于烷烃的高H/C比会导致严重的氢转移过程和大量的轻质烷烃,因此实现起来具有挑战性。本文将CO 2引入到HZSM-5沸石上的环己烷转化过程中,可以提高芳烃选择性。通过优化反应条件,在2.7 MPa (CO 2 )、450 ℃、1.7 h -1条件下,芳烃(苯、甲苯、二甲苯和C 9+)选择性提高到48.2% ,比没有CO 2的情况更好(芳香族选择性= 43.2%)。原位透射傅立叶变换红外光谱表明,在CO 2存在下,在环己烷转化过程中会形成许多含氧化学中间体(例如,羧酸、酸酐、不饱和醛/酮或烯酮) 。13 C同位素标记实验结果表明CO 2可以通过形成含氧化学中间体进入芳烃中,从而提高芳烃选择性。该研究为提高烷烃芳构化过程的芳烃选择性开辟了一条绿色、经济且有前景的途径。