物理化学学报 >> 2002, Vol. 18 >> Issue (05): 432-436.doi: 10.3866/PKU.WHXB20020510

研究论文 上一篇    下一篇

UBI-QEP法研究氧化钴上的催化还原脱硫反应

孙杰;林敬东;易军;魏光;陈鸿博;廖代伟   

  1. 厦门大学化学系,2海洋系,3固体表面物理化学国家重点实验室,4物理化学研究所,厦门　361005
  • 收稿日期:2001-09-27 修回日期:2002-01-31 发布日期:2002-05-15
  • 通讯作者: 廖代伟 E-mail:dwliao@xmu.edu.cn

UBI-QEP Study of Catalytic Reduction Desulfuration on Cobalt Oxide

Sun Jie;Lin Jing-Dong;Yi Jun;Wei Guang;Chen Hong-Bo;Liao Dai-Wei   

  1. Department of Chemistry,2Department of Oceanography,3State Key Laboratory of Physical Chemistry on Solid Surfaces,4Institute of Physical Chemistry,Xiamen University,Xiamen　361005
  • Received:2001-09-27 Revised:2002-01-31 Published:2002-05-15
  • Contact: Liao Dai-Wei E-mail:dwliao@xmu.edu.cn

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摘要： 应用UBIQEP能学方法,研究了氧化钴表面上的催化还原脱硫反应. 发现在CO还原SO2的过程中,低温条件下,反应遵循氧化还原（Redox）机理,即CO先与晶格氧反应在表面产生氧缺位,然后SO2在氧阴离子空穴上被还原;在高温条件下,COS中间态确实存在,反应为Redox机理和COS中间态机理共同作用.中间产物SO是极不稳定的,即能很快被CO继续还原,又可以为表面氧物种所氧化.COS可抑制表面氧物种,因此能起到间接控制该反应的作用.

关键词: 脱硫, 单位键指标-二次指数势(UBIQEP)能学, 氧化钴, 催化还原, 烟道气

Abstract: The catalytic reduction desulfuration on cobalt oxide was investigated using UBIQEP method.It was found that the reaction followed the Redox mechanism in the reduction process of SO2 with CO at low temperature.First,the carbon monoxide reacted with lattice oxygen and produced oxygen vacancy on the surface.Then,the SO2 was reduced on the vacancy of oxygen anion.At high temperature,however,there was intermediate COS.Therefore,the reaction followed both the Redox mechanism and the COS intermediate mechanism.The intermediate product,SO,is much unstable which can be reduced by CO rapidly and can be oxidized by surface oxygen species.The COS can inhibit the surface oxygen species that can influence the reaction.

Key words: Desulfuration, UBI-QEP(the unity bond indexquadratic potential)Energytics, Cobalt oxide, Catalytic reduction, Flue gas