文献类型：期刊文献

中文题名：炭载Pt基催化剂上甘油氧化反应路径的探究

英文题名：Reaction Pathways for Glycerol Oxidation over Carbon Nanotubes Supported Pt Based Catalysts

作者：董华[1];雷佳契[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：2016

卷号：32

期号：3

起止页码：217

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2014】；CSCD:【CSCD_E2015_2016】；

语种：中文

中文关键词：甘油氧化;炭载Pt基催化剂;反应路径

外文关键词：glycerol oxidation; carbon nanotubes supported Pt based catalysts; reaction pathway

摘要：结合透射电镜(TEM)和X射线光电子能谱(XPS)等表征技术,比较研究了碳纳米管(CNTs)负载的单金属Pt和双金属Pt-Sb催化剂的结构及其非碱性条件下催化甘油氧化反应的性能与路径。结果表明:Sb的引入对催化剂的粒径以及Pt电子性质的影响较小,但Sb可能选择性沉积在Pt原子表面形成空间位阻,控制甘油的转化向有利于其仲羟基氧化的方向进行,从而改变了反应的选择性和路径。Pt/CNTs催化剂主要选择性氧化甘油的伯羟基生成甘油醛(GLyD)和甘油酸(GLYA),GLYA再进一步氧化生成羟基丙酮酸(HPYA)和亚酒石酸(TA);Pt-Sb/CNTs催化剂则优先氧化甘油的仲羟基生成二羟基丙酮(DHA),DHA进一步氧化生成HPYA;两种反应路径下生成的HPYA和TA最终都会氧化断键生成乙醇酸(GLYCA)等产物。
Comparative studies of the structure and catalysis of the oxidation of glycerol over Pt/CNTs and Pt-Sb/CNTs catalysts under base-free conditions were performed and the corresponding possible reaction pathways were proposed by using the transmission electron microscopy（TEM）,X-ray photoelectron spectroscopy（XPS） and other characterization techniques.The addition of Sb to the catalyst has been found to have almost no effects on the particle size and electronic properties of Pt.However,Sb may be selectively deposited on the surface of Pt atom and sterically control the conversion of glycerol in an orientation favorable to its secondary hydroxyl group,thus changing the selectivity of the reaction path.The monometallic Pt/CNTs catalyst preferred to oxide the primary hydroxyl groups of glycerol,generating glyceraldehyde（GLYD） and then glyceric acid（GLYA）,which was further oxidized into hydroxypyruvic acid（HPYA） and tartronic acid（TA）,while the bimetallic Pt-Sb/CNTs catalyst favored for the oxidation of the secondary hydroxyl group of glycerol,generating dihydroxyacetone（DHA） and was further transformed into HPYA.Both the produced HPYA and TA during the two reaction routes could eventually be oxidized to glycolic acid（GLYCA） and other products by the cleavage of C-C bond.