载体酸性对Pt/USY菲加氢制烷基金刚烷的影响  

Effect of support acidity on hydrogenation of phenanthrene to alkyl adamantane over Pt/USY catalysts

作　　者：王学明 李晓红[1] 李文英[1] WANG Xueming;LI Xiaohong;LI Wenying(State Key Laboratory of Clean and Efficient Coal Utilization,Key Laboratory of Coal Science and Technology(Taiyuan University of Technology),Ministry of Education,Taiyuan 030024,Shanxi,China)

机构地区：[1]太原理工大学省部共建煤基能源清洁高效利用国家重点实验室,煤科学与技术教育部重点实验室,山西太原030024

出　　处：《化工学报》2021年第10期5196-5205,共10页CIESC Journal

基　　金：国家自然科学基金项目(22038008);中国神华煤制油化工有限公司科技创新项目(MZYHG-2021-01);山西省自然科学基金项目(201901D111083)。

摘　　要：以Pt为活性组分、经不同浓度草酸铝处理的USY分子筛为载体,制备了Pt/USY催化剂,并用于菲一步加氢饱和反应和加氢异构反应体系。由于金属活性位点Pt上易发生加氢反应,USY载体酸性位点上易发生异构反应和裂解反应,实验分别考察了Pt颗粒、载体的酸强度和酸量对菲转化率和产物分布的影响。结果表明,活性金属Pt颗粒尺寸及分散度直接影响菲加氢饱和产物分布;草酸处理后制备的催化剂Pt/0.05-USY、Pt/0.1-USY较未经酸处理的Pt/USY更利于菲加氢反应。全氢蒽是菲向目标产物烷基金刚烷转化的关键中间产物,异构产物烷基金刚烷生成需在USY分子筛Brφnsted酸位点完成;随着催化剂载体酸量和酸强度的降低,裂解反应程度迅速减弱;菲加氢反应最终产物以加氢饱和反应产物为主;使用Pt/0.1-USY催化剂异构反应产物烷基金刚烷收率为2.3%。Pt/USY catalysts were prepared by using Pt as the active component and USY zeolite treated with different concentrations of oxalic acid as supports.For the investigation of concurrent hydrogenation saturation and isomerization,phenanthrene was chosen as a model compound.Since the hydrogenation reaction is prone to occur on the metal active site Pt and the isomerization reaction and cleavage reaction are prone to occur on the acid site of the USY carrier,the influence of the strength and concentration of acid sites on the phenanthrene conversion and product distribution was investigated.The particle size and dispersion of Pt sites affect the conversion rate of phenanthrene,which is faster over Pt/0.05-USY and Pt/0.1-USY than over Pt/USY catalysts.Perhydroanthracene is the key intermediate in the hydrogenation of phenanthrene to alkyl adamantane.The Brφnsted acid sites of the support promote the isomerization of alkyl adamantane.The formation of the isomer alkyl adamantane needs to be completed at the Br?nsted acid site.While decreasing the content and the strength of acid site in USY,the cracking reaction is inhibited which enhances the phenanthrene hydrogenation reaction to yield more hydrogenation saturated products.The yield of alkyl amantadane was 2.3%using Pt/0.1-USY catalysts.

关 键 词：催化作用 加氢反应 异构反应 分子筛 裂解反应 

分 类 号：O643.32[理学—物理化学]