高等学校化学学报

高等学校化学学报 ›› 2002, Vol. 23 ›› Issue (5): 919.

• 研究论文 • 上一篇    下一篇

激光促进Pb和Bi磷酸盐表面上异丁烷氧化脱氢反应

钟顺和, 耿云峰, 陶跃武   

  1. 天津大学化工学院, 天津 300072
  • 收稿日期:2000-11-20 出版日期:2002-05-24 发布日期:2002-05-24
  • 通讯作者: 钟顺和(1938年出生),男,教授,博士生导师,主要从事工业催化剂设计等研究.
  • 基金资助:

    国家自然科学基金(批准号:29773031)资助.

Laser Stimulated Oxidative Dehydrogenation of Isobutane to Isobutene on the Surface of Pb and Bi Phosphate

ZHONG Shun-He, GENG Yun-Feng, TAO Yue-Wu   

  1. College of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
  • Received:2000-11-20 Online:2002-05-24 Published:2002-05-24

PDF (PC)

被引次数

7

摘要： 采用沉淀法制备了Pb3(PO4)2和BiPO4固体材料,用XRD,IR,TPD和LSSR等手段对Pb3(PO4)2和BiPO4的晶体结构、表面构造、化学吸附性能和激光促进异丁烷氧化脱氢反应性能进行了研究.结果表明,固体材料表面由Lewis碱位P＝O和P-O-M(Pb或Bi)键中的O2-及Lewis酸位Pb2+或Bi3+构成;异丁烷分子中两个甲基中的H分别吸附在两个相邻的Lewis碱位P＝O上,形成双位分子吸附态;在常压和200℃条件下,用一定频率的激光激发固体表面P＝O键,发生异丁烷氧化脱氢反应,产物异丁烯的选择性大于95%,在激光促进表面反应体系中,激光能量的利用率主要取决于固体材料的振动结构和对反应物分子的吸附能力,反应产物的选择性主要决定于反应物分子在固体表面上的吸附态.

关键词: 激光促进表面反应, 磷酸盐, 氧化脱氢, 异丁烷, 异丁烯

Abstract: Pb3(PO4)2 and BiPO4 were prepared by the precipitation method.The surface composition, structure, chemisorption properties and the behavior of laser stimulated isobutane selective oxidation were investigated by means of the techniques of XRD, IR, TPDand LSSR.The results showed that both Lewis base sites, O2- on the surface P＝O　or Pb(Bi)—O bonds, and Lewis acid site, Pb2+ or Bi3+ appear on the surface of Pb3(PO4)2 or BiPO4. Two methyl hydrogens in isobutane molecule can be chemisorbed at the terminal oxygen of neighboring Lewis base sites P＝O bonds on the surface of phosphate.Under the conditions of 0.1 MPa and 200 with the 1056 cm-1 laser photons exciting the P＝O bonds for 1000 times, the oxidative dehydrogenation reaction of isobutane occurred remarkably with the product selectivity of isobutene over 95%.In the course of LSSR, the conversion of isobutane depends on the vibrational structure of the solid materials and the adsorbing amount of is obutane on the excited P ＝O bonds, the selectivity of the reaction product depends on the adsorbing state of isobutane on the solid surface.

Key words: Laser stimulated surface reaction, Phosphate, Oxidative dehydrogenation, Isobutane, Isobutene

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