Citation: ZHANG Shuan-Qin, KONG Ling-Dong, ZHAO Xi, Roel JANSEN, CHEN Jian-Min. Effects of Ammonia and Amines on Heterogeneous Oxidation of Carbonyl Sulfide on Hematite[J]. Acta Physico-Chimica Sinica, ;2013, 29(09): 2027-2034. doi: 10.3866/PKU.WHXB201306171 shu

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

1.
Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, P. R. China

Received Date: 22 March 2013
Available Online: 17 June 2013
Fund Project: 国家自然科学基金(21077025, 21277028, 21190053) (21077025, 21277028, 21190053)上海市科学技术委员会项目(10231203801, 10JC1401600)资助 (10231203801, 10JC1401600)

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 (CO₃^2-), and surface SO₄^2-. 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.
- Carbonyl sulfide,
- Ammonia,
- Amine,
- Hematite,
- Heterogeneous reaction
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