碳硅复合材料负载金钯合金在无碱水相中催化苯甲醇氧化
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- 英文论文题名：Benzyl alcohol oxidations in base-free aqueous solutions using Au–Pd alloy nanoparticle catalysts on carbon-silica composites
- 论文作者：郭启水 ; 万颖
- 英文论文作者：Qishui Guo ; Ying Wan ; Shanghai Normal University
- 年：2016
- 作者机构：上海师范大学;
- 论文关键词：金钯合金 ; 有序介孔 ; 碳硅载体 ; 苯甲醇氧化 ; 无碱水相
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第三十三分会：绿色化学
- 语种：中文
- 分类号：O643.36
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第三十三分会 ; 绿色化学
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：220k
- 原文格式：D
- 会议级别：全国
摘要
金钯合金催化剂由于双金属间电子转移等原因比单金属催化剂在醇类选择氧化、饱和碳氢键活化、双氧水制备等反应中表现出更为优越的催化活性和产物选择性,但传统通过沉积沉淀法、溶胶法等后负载方法制备的金钯合金催化剂存在易团聚、易流失等缺点。我们通过通过多元共组装的方法制备负载有金钯的碳硅复合材料催化剂,载体中含有的巯基使金和钯离子均匀分布在载体中,经过焙烧还原后,形成大小均一的金钯合金粒子镶嵌在孔墙中,可以有效防止纳米粒子的团聚和流失。醇类的氧化是化工行业中重要的反应,但大部分的催化剂在催化醇类氧化时需要在有碱或有机溶剂中进行反应。我们合成的金钯合金催化剂在无碱水相中对苯甲醇具有良好的催化活性,通过添加巯基捕获实验、重复实验,表明催化剂也具有很好的稳定性,更加符合绿色化学的要求。通过苯甲醇氧化结果和XRD、XPS、TEM、EDS等多种表征方法结合,从晶格间距、电荷转移、原子键能等方面对金钯合金的形成以及催化机理有了更加深入的了解。
It has been demonstrated that bimetallic catalysts have a significant enhancement in activity and selectivity compared with monomatellic catalysts. But the traditional alloy catalyst prepared by the post load method is easy to reunite, leaching and so on, and the specific mechanism of the alloy catalyst still needs further exploration. Here, we report a stable and efficient ordered mesoporous silica-carbon supported Au-Pd alloy catalysts. The catalysts have a great conversion for benzyl alcohol oxidation in base-free aqueous solutions, and with the different mole ratio of gold and palladium have different properties. When the mole ratio is 1:1, the catalysts have the highest activity. In order to further explore the catalytic mechanism of alloy, in this work by XRD, TEM, XPS and EDS technology on the material have been characterized.
It has been demonstrated that bimetallic catalysts have a significant enhancement in activity and selectivity compared with monomatellic catalysts. But the traditional alloy catalyst prepared by the post load method is easy to reunite, leaching and so on, and the specific mechanism of the alloy catalyst still needs further exploration. Here, we report a stable and efficient ordered mesoporous silica-carbon supported Au-Pd alloy catalysts. The catalysts have a great conversion for benzyl alcohol oxidation in base-free aqueous solutions, and with the different mole ratio of gold and palladium have different properties. When the mole ratio is 1:1, the catalysts have the highest activity. In order to further explore the catalytic mechanism of alloy, in this work by XRD, TEM, XPS and EDS technology on the material have been characterized.
引文
[1]Wang,S.;Wang,J.;Zhao,Q.;Li,D.;Wang,J.-Q.;Cho,M.;Cho,H.;Terasaki,O.;Chen,S.;Wan,Y.ACS Catalys,2015,5,797.
[2]Wang,S.;Zhao,Q.;Wei,H.;Wang,J.Q.;Cho,M.;Cho,H.S.;Terasaki,O.;Wan,Y.Journal of the American Chemical Society,2013,135,11849.
[2]Wang,S.;Zhao,Q.;Wei,H.;Wang,J.Q.;Cho,M.;Cho,H.S.;Terasaki,O.;Wan,Y.Journal of the American Chemical Society,2013,135,11849.