Cracking(desulfurization)behavior of hugh boiling point organic sulfur compounds over zeolite catalysts

本课题研究了噻吩和苯并噻吩等有机含硫化合物在沸石及相关材料负载贵金属加氢脱硫反应中的加氢裂化（加氢脱硫）行为，以期开发新型高活性沸石基石油加氢脱硫催化剂。噻吩类化合物对沸石、柱状粘土和介孔硅酸盐负载的铂具有较高的加氢脱硫活性。沸石材料负载Pt对噻吩类化合物的加氢脱硫具有较高的催化活性，其活性高于CoMo/A1203型工业加氢脱硫催化剂。这表明，在沸石材料上负载Pt作为石油加氢脱硫的新型催化剂是有可能的。通过对噻吩类化合物吸附在沸石及相关材料上的动力学和光谱分析，发现噻吩类化合物在沸石材料的酸位上被活化，氢在Pt上被活化形成外溢氢。Pt上形成的溢出氢攻击沸石材料酸位上的活性噻吩化合物，加氢脱硫反应顺利进行。在本课题研究成果的基础上，为设计第二代高活性石油加氢脱硫催化剂提供了一定的可能性。

In this research project, the hydrocracking (hydrodesulfurization) behavior of organic sulfur compounds such as thiophene and benzothiophene in the hydrodesulfurization reaction over noble metals supported on zeolites and related materials was investigated in order to develop new highly active zeolite-based hydrodesulfurizarion catalysts for peiroleum. The thiophene compounds showed high hydrodesulfurizarion reactivities over Pt supported on zeolite, pillared clays and mesoporous silicates. The Pt supported on zeolitic materials indicated high catalytic activities for the hydrodesulfurization of thiophene compounds and their activities were higher than that of CoMo/A1203 commercial hydrodesulfurization catalysts. This implies that there is a possibility for the usage of Pt supported on zeolitic materials as new hydrodesulfurization catalysts for petroleum.By the kinetic and spectroscopic analysis of thiophene compounds adsorbed on zeolites and related materials, it was revealed that thiophene compounds are activated on acid sites of these zeolitic materials and hydrogen is activated on Pt to form spillover hydrogen. The spillover hydrogen formed on Pt attacks the activated thiophene compounds on acid site of zeolitic materials and the hydrodesulfurizationn reaction proceeds smoothly.On the basis of results obtained in this research project, there are some possibilities to design second generation highly active hydrodesulfurization catalysts for petroleum.