Pt/Mn-silicalite-1催化剂的制备及丙烷脱氢性能  

Preparation of Pt/Mn-silicalite-1 Catalysts and Their Catalytic Performance for Propane Dehydrogenation

作　　者：刘奕萱 胡慧敏 范晓强 于学华 孔莲 肖霞 解则安 赵震 LIU Yixuan;HU Huimin;FAN Xiaoqiang*;YU Xuehua;KONG Lian;XIAO Xia;XIE Zean;ZHAO Zhen(School of Chemistry and Chemical Engineering,Shenyang Normal University,Shenyang 110034,China;State Key Laboratory of Heavy Oil Processing,China University of Petroleum,Beijing 102249,China)

机构地区：[1]沈阳师范大学化学化工学院,沈阳110034 [2]中国石油大学(北京),重质油国家重点实验室,北京102249

出　　处：《高等学校化学学报》2025年第3期72-80,共9页Chemical Journal of Chinese Universities

基　　金：国家自然科学基金(批准号:22172101);辽宁省应用基础研究计划项目(批准号:2023JH2/101600059);辽宁省“兴辽英才”青年拔尖人才计划(批准号:XLYC2203138);辽宁省属本科高校基本科研业务费专项资金项目(批准号:LJ212410166046);沈阳师范大学重大项目孵化工程项目资助。

摘　　要：丙烷作为天然气、页岩气等的重要组成成分,其高效催化转化不仅具有重要的理论研究意义,而且具有广阔的应用前景.丙烷直接脱氢制丙烯已成为目前增产丙烯的重要手段之一,提高Pt基催化剂的稳定性、降低贵金属Pt的用量是该反应的关键点.本文设计和制备了不同过渡金属Mn掺杂量的Silicalite-1(S-1)分子筛(xMn-S-1)载体,并负载活性组分Pt制备了一系列Pt/x Mn-S-1催化剂.利用扫描电子显微镜(SEM)、X射线衍射仪(XRD)、拉曼光谱仪(Raman)和紫外-可见漫反射光谱仪(UV-Vis DRS)等手段对催化剂进行了表征,并对其进行了丙烷脱氢性能评价.结果表明,乙二胺四乙酸二钠(EDTA)配位后的Mn物种进入S-1分子筛的骨架中形成Mn-O-Si物种,该物种可以有效锚定Pt,从而使Pt物种以高分散的形式存在.通过活性评价结果可知,Pt/0.05Mn-S-1催化剂表现出最佳的丙烷催化脱氢性能,其丙烷初始转化率为51.9%,反应6 h后仍保持在36.7%.这可能是由于适量Mn的掺杂使载体Mn-S-1与活性组分Pt之间产生了强相互作用所致,从而提高了Pt/0.05Mn-S-1的丙烷脱氢活性及稳定性.As one of the important components of natural gas and shale gas,the catalytic conversion of propane not only has important theoretical research significance but also has broad prospects in application.Propane dehydrogenation is one of the important ways to enhance the production of propylene,and the key of this reaction is to improve the stability of Pt-based catalysts and minimize the amount of Pt.In this work,the Mn-doped silicalite-1(S-1)supports(x Mn-S-1)with different Mn doping amounts were designed,and prepared a series of Pt/x Mn-S-1 catalysts was prepared by loading Pt.The scanning electron microscope(SEM),X-ray diffraction(XRD),Raman spectra and ultraviolet-visible diffuse reflectance spectroscopy(UV-Vis DRS)characterizations were carried out,and the catalytic performance was tested for propane dehydrogenation.According to the characterizations,the Mn species enter the framework of S-1 to form Mn-O-Si by coordinating with EDTA,which can anchor the Pt species to form highly dispersed Pt species.According to the activity evaluation,Pt/0.05Mn-S-1 catalyst showed the best dehydrogenation performance with the propane initial conversion of 51.9%.And the propane conversion was 36.7%after 6 h reaction.The reason may be the strong interaction formed between the Mn-S-1 support and active metal Pt with the appropriate amount of Mn doping,which results in the enhanced propane dehydrogenation activity and stability over Pt/0.05Mn-S-1 catalyst.

关 键 词：丙烷脱氢 丙烯 Mn-silicalite-1载体 浸渍合成 

分 类 号：O643.3[理学—物理化学]