催化学报

催化学报 ›› 2008, Vol. 29 ›› Issue (10): 1009-1014.

• 研究论文 • 上一篇    下一篇

负载型金催化剂催化乙醇选择氧化反应

成艳,李钢,马书启,王祥生,陈永英   

  1. 大连理工大学催化化学与工程系精细化工国家重点实验室, 辽宁大连 116012
  • 收稿日期:2008-10-25 出版日期:2008-10-25 发布日期:2008-10-25

Selective Oxidation of Ethanol over Supported Gold Catalysts

CHENG Yan, LI Gang*, MA Shuqi, WANG Xiangsheng, CHEN Yongying   

  1. State Key Laboratory of Fine Chemicals, Department of Catalytical Chemistry and Engineering, Dalian University of Technology, Dalian 116012, Liaoning, China
  • Received:2008-10-25 Online:2008-10-25 Published:2008-10-25

PDF

1199

被引次数

16

摘要： 选择不同氧化物(Al2O3, SiO2, TiO2, MgO)和H-ZSM-5分子筛作为载体,以尿素为沉淀剂,采用沉积-沉淀法制备了一系列负载型金催化剂. 采用X射线衍射、电感耦合等离子体发射光谱、程序升温还原、NH3程序升温脱附和透射电镜等技术对催化剂样品进行了表征,并测定了催化剂对乙醇选择氧化反应的催化性能. 选择Au/Al2O3催化剂,考察了金负载量、反应条件(温度、压力、时间)和添加剂对乙醇选择氧化反应的影响. 结果表明,所制备的Au/Al2O3催化剂的金负载率较高,金粒子较小(3～4 nm)且分布均匀. 载体对金催化剂催化乙醇氧化反应有显著影响,主要产物为乙醛、乙酸乙酯和缩醛. 以TiO2为载体时,乙醇转化率较高. 以Al2O3为载体时,乙酸乙酯选择性较高; 少量碱性添加剂可抑制缩醛的生成,并可提高乙醇转化率和乙酸乙酯选择性. 在优化的条件下,乙醇转化率可达4.7%, 乙酸乙酯选择性可达93.5%.

关键词: 沉积-沉淀法, 金, 氧化铝, H-ZSM-5分子筛, 氧化硅, 氧化钛, 氧化镁, 负载型催化剂, 乙醇, 选择氧化

Abstract: The gold catalysts supported on several oxides and H-ZSM-5 were used in the se lective oxidation of ethanol. Au/Al2O3 catalyst gave the highest selectivity for acetic ester. An appropriate quantity of basic additive in the reaction sys tem could evidently increase the ethanol conversion and the selectivity for acet ic ester. The ethanol conversion was 4.7% with 93.5% selectivity for acetic es ter under the optimal conditions.

Key words: deposition-precipitation, gold, alumina, H-ZSM-5 zeolite, silica, titania, magnesia, supported catalyst, ethanol, selective oxidation