Acta Phys. -Chim. Sin. ›› 2013, Vol. 29 ›› Issue (09): 2027-2034.doi: 10.3866/PKU.WHXB201306171

• CATALYSIS AND SURFACE SCIENCE • Previous Articles     Next Articles

Effects of Ammonia and Amines on Heterogeneous Oxidation of Carbonyl Sulfide on Hematite

ZHANG Shuan-Qin, KONG Ling-Dong, ZHAO Xi, Roel JANSEN, CHEN Jian-Min   

  1. Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, P. R. China
  • Received:2013-03-22 Revised:2013-06-17 Published:2013-08-28
  • Contact: KONG Ling-Dong, CHEN Jian-Min E-mail:ldkong@fudan.edu.cn;jmchen@fudan.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (21077025, 21277028, 21190053) and Science&Technology Commission of Shanghai Municipality, China (10231203801, 10JC1401600).

Abstract:

The heterogeneous oxidation of carbonyl sulfide (COS) on hematite pre-adsorbed with ammonia and methylamine, trimethylamine, triethylamine, phenylamine, pyridine, and pyrrole was investigated using in situ diffuse-reflectance infrared Fourier-transform spectroscopy (DRIFTS) at room temperature. The products and kinetics of the heterogeneous reaction were investigated. The results showed that adsorbed COS could be oxidized on the surface of hematite pre-adsorbed with these basic substances, forming gaseous carbon dioxide (CO2), surface bicarbonate (HCO3-), surface carbonate (CO32-), and surface SO42-. Ammonia and amines pre-adsorbed on hematite significantly enhanced the reactivity of COS. Hematite with pre-adsorbed methylamine exhibited the highest reactivity, about 4.5 times higher than that of pure hematite, whereas the effects of phenylamine and pyrrole were not obvious. The reaction rates with the basic substances were in the order of methylamine>trimethylamine>ammonia>triethylamine>pyridine> pyrrole> phenylamine≈pure hematite. The basic substances changed the reaction order from first to second. Coverage by the basic substances and surface water also played important roles in the heterogeneous reaction of COS. These experimental results indicated that surface oxygen species (M―O-) were the key factor contributing to oxidizing activities in the presence of basic substances. The heterogeneous oxidation mechanism of COS on hematite with pre-adsorbed basic substances is discussed on the basis of the experimental results.

Key words: Carbonyl sulfide, Ammonia, Amine, Hematite, Heterogeneous reaction

MSC2000: 

  • O647