期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 113, 期 42, 页码 18223-18232出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp9054999
关键词
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资金
- SRF [NCET-05-0608]
- Excellent Young Teachers Program of MOE, PRC, NSFC [20476061]
- State Key Basic Research Program of China [2006CB202505]
- CNPC Science & Technology Innovation Foundation [20090-5006-04-07]
- Graduate Innovative Foundation of China University of Petroleum [S2009-12]
The reaction of SO2 on Ir(111) has been systematically studies using self- consistent periodic density functional therapy. Adsorptions of the reactants, intermediates, and products involved are calculated. In all possible adsorption modes of SO2, the parallel adsorption (eta(1)(S)-eta(1)(O)-eta(1)(O)) is found to be the most favorable. Intermediate SO is also preferable for parallel adsorption. S and O are exclusively adsorbed at 3-fold sites. The oxidation product SO3 has two stable adsorption modes without any preference, i.e., eta(1)(O)-eta(1)(O)-eta(1)(O) (crown) and (eta(1)(S)-eta(1)(O)-eta(1)(O) (chair). In the absence of oxygen, the disproportionated reaction, 3SO(2) -> S + 2SO(3), is initiated by SO2 dissociation into SO and atomic O; then SO quickly decomposes into S and O; and lastly, the O atoms formed in the SO2 and SO dissociation are rapidly exhausted by other SO2. The fast reductions of SO and O accord well with the fact that they were not detected in the experiment [Fujitani, Nakamura, Kobayashi, Takahashi, Haneda, Hamada Surf Sci, 2007, 601, 1615]. Further reaction of SO3 is, expected to take place at high temperatures because of the high energy barriers involved (at least 2,06 eV), also in agreement with the experimental finding.
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