催化学报

催化学报 ›› 2009, Vol. 30 ›› Issue (12): 1215-1221.

• 研究论文 • 上一篇    下一篇

超临界二氧化碳中功能化聚乙二醇稳定的钯纳米粒子催化醇的选择氧化反应

汪向锐1, 冯 博1, 杨汉民2, 侯震山1, 赵秀阁1, 胡 玉1, 乔云香1, 李 欢1, 潘珍燕1   

  1. 1 华东理工大学工业催化研究所, 结构可控先进功能材料及其制备教育部重点实验室, 上海 200237 2 中南民族大学催化材料科学湖北省暨国家民委-教育部共建重点实验室, 湖北武汉 430074
  • 收稿日期:2009-12-25 出版日期:2009-12-25 发布日期:2013-09-29

Functionalized Poly(ethylene glycol)-Stabilized Palladium Nanoparticles for Se-lective Oxidation of Alcohols in Supercritical Carbon Dioxide

WANG Xiangrui1, FENG Bo1, YANG Hanmin2, HOU Zhenshan1,*, ZHAO Xiuge1, HU Yu1, QIAO Yunxiang1, LI Huan1, PAN Zhenyan1   

  1. 1Key Laboratory for Advanced Materials, Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai 200237, China 2Key Laboratory of Catalysis and Materials Science of the State Ethnic Affairs Commission and Ministry of Educa-tion, South-Central University for Nationalities, Wuhan 430074, Hubei, China
  • Received:2009-12-25 Online:2009-12-25 Published:2013-09-29

PDF

1097

被引次数

16

摘要： 以超临界二氧化碳 (scCO2)/聚乙二醇 (PEG) 两相为反应介质, 双齿氮配体功能化聚乙二醇稳定的 Pd 纳米颗粒作为催化剂, 进行了醇的需氧氧化反应. 系统研究了催化剂制备条件和反应条件对苯甲醇需氧氧化反应的影响. 结果表明, 以氢气为还原剂制备的 Pd 纳米粒子的催化活性最高. 反应结束后, 可以利用 scCO2 直接进行原位萃取得到产物, 实现了催化剂与产物的有效分离和催化剂的循环使用. 反应中没有检测到钯的流失. 催化剂经过 5 次循环利用后转化率仍可达 98%.

关键词: 超临界二氧化碳, 聚乙二醇, 醇, 需氧氧化反应, 钯纳米粒子

Abstract: The aerobic oxidation of various alcohols to the corresponding aldehydes or ketones was carried out using stabilized palladium nanoparticles in a supercritical carbon dioxide (scCO2)/poly(ethylene glycol) (PEG-2000) biphasic system. The effects of reaction conditions on catalytic activity were investigated in detail. Among the Pd nano-catalysts reduced with different reductants, Pd nanoparticles obtained by H2 reduction showed the best catalytic performance in the oxidation of benzyl alcohol. The products can be easily extracted with scCO2 in situ from the Pd nano-catalyst immobilized in functionalized poly(ethylene glycol), and therefore the loss of palladium could be eliminated. The conversion reached 98% after the catalyst was reused 5 times.

Key words: supercritical carbon dioxide, poly(ethylene glycol), alcohol, aerobic oxidation, palladium nanoparticle