文献类型：期刊文献

中文题名：有机胺助剂促进的Pt/CNTs催化剂上甘油选择性氧化反应性能

英文题名：Selective Oxidation of Glycerol over Amine Promoted Pt/CNTs Catalysts

作者：严寒[1];马媛媛[1];段学志[1];钱刚[1];周兴贵[1]

机构：[1]华东理工大学化学工程联合国家重点实验室,上海200237

年份：2018

卷号：34

期号：2

起止页码：138

中文期刊名：化学反应工程与工艺

外文期刊名：Chemical Reaction Engineering and Technology

收录：CSTPCD;;Scopus;北大核心:【北大核心2017】；CSCD:【CSCD_E2017_2018】；

基金：上海市自然科学基金项目(17ZR1407500)

语种：中文

中文关键词：甘油选择性催化氧化;碳纳米管负载Pt催化剂;胺助剂

外文关键词：selective catalytic oxidation of glycerol;carbon nanotubes supported Pt catalyst;amine promoters

摘要：为了提高Pt基催化剂上非碱性条件下甘油选择性氧化反应的性能,制备了两种有机胺[二乙胺(DEA)和二乙醇胺(DEOA)]助剂促进的碳纳米管(CNTs)负载的Pt催化剂(Pt/CNTs-DEA和Pt/CNTs-DEOA),考察了DEA和DEOA促进的Pt/CNTs催化甘油选择性氧化反应的性能,并结合高角度环形暗场-扫描透射电子显微镜、X射线光电子能谱以及程序升温脱附-质谱等分析了可能的影响原因,在此基础上研究了反应工艺条件对Pt/CNTs-DEOA催化剂性能的影响。结果表明,DEA和DEOA的引入并未明显改变Pt/CNTs催化剂的粒径,但提高了催化剂表面Pt 4f的结合能以及增强了其碱性位,从而提高了甘油氧化反应的初始速率。尤其是Pt/CNTs-DEOA催化剂,其表面具有更高的Pt 4f结合能以及较强的碱性位,因而不仅表现出较高的初始反应速率,而且表现出较高的甘油醛和C3产物总选择性;但是DEOA添加量过多也会导致催化剂表面较多活性位被覆盖从而降低其活性。此外得到Pt/CNTs-DEOA催化剂上甘油氧化反应较适宜的反应温度为333 K、甘油与Pt的物质的量比为850。
Different amine-promoted Pt/CNTs catalysts were prepared and then tested for selective oxidation of glycerol (GLY) under base-free conditions to probe the promoter effects. The introduction of diethylamine (DEA) and diethanol amine (DEOA) appears to enhance both the initial reaction rate of glycerol oxidation and the selectivity to glyceraldehyde (GLYD), which may be due to the higher binding energy of Pt 4f and stronger basic sites. However, excessive amount of DEOA leads to the blocking of Pt active sites and thus a lower initial reaction rate. Moreover, there exists optimal values for reaction temperature and GLY/Pt molar ratio. The insights revealed here could guide the catalyst rational design and optimization for the selective base-free oxidation of glycerol.