物理化学学报 >> 2001, Vol. 17 >> Issue (10): 936-939.doi: 10.3866/PKU.WHXB20011014

研究简报 上一篇    下一篇

激光促进乙烯在硫酸镍上表面反应

钟顺和;陈崧哲;辛秀兰   

  1. 天津大学化工学院,天津 300072
  • 收稿日期:2001-03-22 修回日期:2001-06-04 发布日期:2001-10-15
  • 通讯作者: 钟顺和 E-mail:shzhong@public.tpt.tj.cn

Laser Stimulated Surface Reaction of C2H4 on Nickel Sulfate

Zhong Shun-He;Chen Song-Zhe;Xin Xiu-Lan   

  1. College of Chemical Engineering and Technology, Tianjin University,Tianjin 300072
  • Received:2001-03-22 Revised:2001-06-04 Published:2001-10-15
  • Contact: Zhong Shun-He E-mail:shzhong@public.tpt.tj.cn

摘要: 制备了硫酸镍固体材料.采用红外光谱(IR)、程序升温脱附(TPD)和激光促进表面反应(LSSR)技术,研究了乙烯在NiSO4表面上的化学吸附态和激光促进C2H4表面反应性能.实验结果表明,C2H4以H原子与固体材料表面Lewis碱位(S=O键中的端氧)作用,形成分子吸附态.在常压和100 ℃条件下,用1079 cm-1激光激发吸附有C2H4分子中H的S=O键100次, C2H4转化率可达15%,生成丁二烯的选择性为100%.根据表征和反应结果,讨论了C2H4在NiSO4上的LSSR机理和影响LSSR性能的因素.

关键词: 激光促进表面反应, 固体材料, 硫酸镍, 乙烯, 丁二烯

Abstract: Solid material NiSO4 was prepared. A TEACO2 laser generator was adopted as the light source to carry on laser stimulated surface coupling reaction of ethylene. The infrared vibration structure and adsorption state of C2H4adNiSO4 system were discussed based on infrared and temperature programmed desorption tests. It was showed that C2H4 is adsorbed as molecular state, bonding with NiSO4 surface through H atom at terminal O of S=O. The 1 079 cm-1 laser was selected to activate solid surfacial bond S=O, which absorbs the photon energy efficiently. At normal pressure and a temperature below 100 ℃, C2H4 conversed to butadiene with a high selectivity of 100%. Increasing laser pulse can improve conversion of C2H4 without change of selectivity. After 200 pulses, C2H4 in the system had been consumed to a large extent, and the product occupied most of the surface active sites, therefore conversion of C2H4 increased at a low speed. Temperature can also affect the laser stimulated surface reaction of C2H4adNiSO4. At 100 ℃, 15.1% of C2H4 convert to butadiene, while keeping high selectivity of 100%. Based on the above experimental results, a mechanism of LSSR was proposed for the conversion of C2H4 to C4H6.

Key words: Laser stimulated surface reaction, Solid material, Nickel sulfate,  Ethylene, Butadiene