不同反应温度下甲苯歧化催化剂表面性质变化及其积炭行为研究  

Study of the Effects of Varying Reaction Temperatures on Surface Properties and Coking Behavior of Toluene Disproportionation Catalysts

作　　者：侯敏 吴雅楠 祁晓岚 李经球 孔德金 HOU Min;WU Yanan;QI Xiaolan;LI Jingqiu;KONG Dejin(State Key Laboratory of Green Chemical Engineering and Industrial Catalysis,SINOPEC Shanghai Research Institute of Petrochemical Technology Company Limited,Shanghai 201208,China)

机构地区：[1]绿色化工与工业催化全国重点实验室,中石化(上海)石油化工研究院有限公司,上海201208

出　　处：《化学反应工程与工艺》2024年第3期202-210,共9页Chemical Reaction Engineering and Technology

基　　金：中国石油化工股份有限公司项目(418024-1)。

摘　　要：探究了纯甲苯歧化反应中,不同反应温度下催化剂表面性质及其积炭行为的差异。采用X射线粉末衍射(XRD)、N_(2)吸附脱附、氨气程序升温脱附(NH_(3)-TPD)、吡啶吸附红外光谱(Py-IR),对在不同反应温度和运行时长下催化剂的结构及表面酸性质的变化进行了表征。同时,采用热重分析(TGA)和全二维色谱(GC×GC)对不同反应温度下催化剂中的积炭行为进行了具有空间分辨性的定量研究。发现催化剂孔道内的可溶性积炭量明显高于外表面的可溶性积炭量,并且相比于375℃时,350℃下反应后催化剂中形成的积炭更少。相应地,催化剂在350℃的纯甲苯歧化反应中,也具有更好的稳定性。The study investigated the differences in surface properties of catalysts and their coking behavior under various reaction temperatures in the pure toluene disproportion reaction.The structural and surface acidity changes of the catalysts at different reaction temperatures and durations were characterized using X-ray powder diffraction(XRD),N_(2) adsorption-desorption isotherms,NH_(3) temperature-programmed desorption(NH3-TPD),and pyridine adsorption infrared spectroscopy(Py-IR).Additionally,thermogravimetric analysis(TGA)and comprehensive two-dimensional gas chromatography(GC×GC)were utilized to conduct spatially resolved quantitative research on the coking behavior within the catalysts at different reaction temperatures.It was found that the amount of soluble coke within the catalysts pores was significantly higher than that on the external surface.Moreover,compared to the reaction at 375℃,the catalyst reacting at 350℃formed less coke.Consequently,the catalyst exhibited better stability during the pure toluene disproportionation reaction at 350℃.

关 键 词：甲苯歧化 积炭 孔道 催化剂 全二维色谱 

分 类 号：O643.36[理学—物理化学]