硫化温度对油溶性催化剂硫化程度的影响  

Effect of Sulfurization Temperature on the Sulfurization Degree of Oil-Soluble Catalysts

作　　者：苏凯宁 张馨月 张晓 周志远 徐春明[2] 胡长禄 徐华 SU Kaining;ZHANG Xinyue;ZHANG Xiao;ZHOU Zhiyuan;XU Chunming;HU Changlu;XU Hua(Petrochemical Research Institute,CNPC,Beijing 102206,China;State Key Laboratory of Heavy Oil Processing,China University of Petroleum,Beijing 102249,China)

机构地区：[1]中国石油石油化工研究院,北京102206 [2]中国石油大学(北京)重质油国家重点实验室,北京102249

出　　处：《石油学报（石油加工）》2024年第3期670-680,共11页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：中国石油科技项目(2020B-2011)基金资助。

摘　　要：针对含硫和不含硫的2种油溶性催化剂在不同硫化温度下进行预硫化处理,采用元素分析、XRD、HRTEM、XPS等手段对处理后的催化剂进行表征,并以二苯并噻吩作为模型化合物,考察不同硫化温度催化剂对二苯并噻吩的脱硫活性和加氢脱硫(HDS)反应路径的影响。结果表明,随着硫化温度的升高,2种油溶性催化剂的Mo^(4+)含量均增加,硫化程度加深,MoS_(2)活性相的XRD特征峰呈现出逐渐尖锐和明显的趋势,且MoS_(2)条纹的长度及堆积层数逐渐增加。在HDS反应性能评价中,2种油溶性催化剂对二苯并噻吩的脱硫性能均以直接脱硫(DDS)路径为主,且随着硫化温度的增加,HDS路径选择性呈现下降趋势。其中,含硫的油溶性催化剂随着硫化温度的升高,其活性呈现下降趋势;而不含硫的油溶性催化剂在硫化温度为320℃时表现出最高的催化活性。Two kinds of oil-soluble sulfur-containing and sulfur-free catalysts are pre-sulfurized at different sulfurization temperatures.The treated catalysts were characterized by elemental analysis,XRD,HRTEM and XPS.Additionally,the effect of catalysts under different sulfurization temperature on the desulfurization activity and hydrodesulfurization(HDS)reaction path of dibenzothiophene were investigated using dibenzothiophene as the model compound.The results show that with the increase of sulfidation temperature,the Mo^(4+)content and the degree of sulfidation for the two oil-soluble catalysts are increased,a gradual sharp and obvious trend in XRD characteristic peaks of MoS_(2)active phase are observed.Moreover,the length of MoS_(2)stripes and the number of stacked layers are gradually increased.In the evaluation of HDS reaction performance,the desulfurization performance of the two oil-soluble catalysts for dibenzothiophene is dominated by the direct desulfurization(DDS)pathway,and the HDS path selectivity shows a decreasing trend with the increase of sulfurization temperature.The activity of oil-soluble catalyst containing sulfur shows a decreasing trend with the increase of sulfurization temperature,while the oil-soluble sulfur-free catalyst exhibits the highest catalytic activity at the sulfurization temperature of 320℃.

关 键 词：油溶性催化剂 硫化温度 MoS 2 加氢脱硫 硫化程度 

分 类 号：TE626[石油与天然气工程—油气加工工程]