| 廖卫平,李扬,赵星岭,金明善,吕宏缨.AuPd/SiO2催化剂用于无溶剂条件下分子氧液相氧化甲苯[J].分子催化,2016,30(4):338-345 |
| AuPd/SiO2催化剂用于无溶剂条件下分子氧液相氧化甲苯 |
| AuPd/SiO2 Catalyst for Selective Solvent-Free Oxidation of Toluene by Dioxygen |
| 投稿时间：2016-04-29 修订日期：2016-06-03 |
| DOI： |
| 中文关键词: AuPd双金属催化剂，选择氧化，甲苯 |
| 英文关键词:Au-Pd bimetallic catalyst selective oxidation toluene |
| 基金项目:国家自然科学基金项目（面上项目，2127319） |
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| 摘要点击次数: 1186 |
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| 中文摘要: |
| 采用浸渍法和溶胶负载法制备了一系列Au-Pd双金属催化剂，用氮吸附法，X光粉末衍射（XRD）、程序升温还原(TPR)，扫描电镜(SEM)和X射线光电子能谱(XPS)对催化剂进行了表征。以分子氧为氧化剂，在无任何其它溶剂存在的条件下，考察了催化剂制备方法、不同类型载体、Au/Pd原子比、浸渍顺序、活化温度、催化剂用量及反应时间等多种因素对甲苯选择氧化反应的影响。实验结果表明：对SiO2载体，以浸渍法制备的催化剂活性较好；而对TiO2载体，以溶胶负载法制备的催化剂活性较好；AuPd双金属催化剂比单金或者单钯催化剂具有更好的催化活性。其中AuPd/SiO2催化剂使甲苯转化率达到56.8%，苯甲酸苄酯的选择性为91.3%，TON值为3692。AuPd/SiO2催化剂中氧化态的钯和零价金更利于催化剂中的电子传递从而利于催化氧化反应的进行。 |
| 英文摘要: |
| A series of Au-Pd bimetallic catalysts were prepared respectively by modified impregnation and sol immobilization methods. In order to study the textural, structural and redox properties, the samples were characterized by nitrogen adsorption, X-ray diffraction (XRD), temperature-programmed reduction (TPR), scanning electro microscope (SEM) and X-ray electron spectroscopy(XPS). The effects of preparation methods, different supporters, atomic ratio of Au/Pd, impregnation sequence and activation temperature on the activity for solvent-free toluene oxidation with dioxygen were investigated. The results showed that, for impregnation method, the catalysts supported by SiO2 represents better catalytic performance. For sol immobilization method, TiO2 is the preferable support. AuPd bimetallic catalysts presents better activity than monometallic catasysts. AuPd/SiO2 is an effective catalyst exhibiting 56.8% conversion of toluene, 91.3% selectivity to benzylbenzoate and the TON values can be achieved 3692. Au0 and PdO are the active phases in AuPd/SiO2 catalyst, these phases seem to be beneficial to the electron transfer and in favour of the activity of the catalyst. |
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