催化学报 ›› 2007, Vol. 28 ›› Issue (3): 281-286.

• 研究论文 • 上一篇    

甲醇水相重整制氢原位还原苯乙酮制备α-苯乙醇

姜莉,祝一锋,项益智,李小年   

  1. 浙江工业大学工业催化研究所, 绿色化学合成技术国家重点实验室培育基地, 浙江杭州 310032
  • 收稿日期:2007-03-25 出版日期:2007-03-25 发布日期:2007-03-25

In-Situ Reduction of Acetophenone to α-Phenylethanol with Hydrogen Derived from Aqueous-Phase Reforming of Methanol

JIANG Li, ZHU Yifeng, XIANG Yizhi, LI Xiaonian*   

  1. State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Institute of Industrial Catalysis, Zhejiang University of Technology, Hangzhou 310032, Zhejiang, China
  • Received:2007-03-25 Online:2007-03-25 Published:2007-03-25

摘要: 在液相状态下,吸热的甲醇水相重整制氢反应和放热的苯乙酮液相加氢反应可使用相同类型 的催化剂,并在相近的反应温度和压力条件下进行. 据此,提出利用甲醇水相重整制氢原位还 原苯乙酮制备α-苯乙醇,将两个反应偶合形成一种新的苯乙酮加氢还原方法,即苯乙酮液相 原位加氢还原法. 通过这种偶合,在Raney Ni催化剂作用下实现了羰基的高选择性还原(α- 苯乙醇选择性可达95%), 同时水相重整过程中甲醇的转化率和氢的选择性也得到明显提高. 实验结果表明,反应条件是影响苯乙酮原位加氢反应性能的重要因素; 优化反应的温度、压 力、苯乙酮浓度和原料配比可以提高甲醇水相重整制氢选择性和羰基加氢选择性.

关键词: 液相, 甲醇, 重整, 苯乙酮, 加氢, 苯乙醇, 偶合, Raney镍

Abstract: Endothermic aqueous-phase reforming of methanol for hydrogen generation and exothermic hydrogenation of acetophenone to α-phenylethanol can be performed over the same type of catalyst under similar conditions (temperature and pressure). In the present work, a novel route for in-situ aqueous-phase hydrogenation of acetophenone to α-phenylethanol was proposed, in which active hydrogen was obtained directly from aqueous-phase reforming of methanol. The experimental results indicated that high selectivity for C=O bond hydrogenation (95% of α-phenylethanol selectivity) was reached. Furthermore, the conversion of methanol and the selectivity for hydrogen in the aqueous-phase reforming of methanol were significantly increased. Also, the optimization of reaction conditions, such as reaction temperature, reaction pressure, acetophenone concentration, and the ratio of raw materials, was performed to promote the selectivity for hydrogen in aqueous-phase reforming of methanol and for α-phenylethanol in acetophenone hydrogenation.

Key words: aqueous phase, methanol, reforming, acetophenone, hydrogenation, phenylethanol, coupling, Raney nickel