期刊
CHEMICAL ENGINEERING JOURNAL
卷 429, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.132376
关键词
Catalytic oxidation; Desulfurization; Phosphorus; Liquid phase; Reaction mechanism
资金
- National Natural Science Foundation of China [22006058, 51968034, 21876071]
- National Key Research and Development Program of China [2018YFC0213400]
- Scientific Research Foundation of Yunnan Province Education Department [2021J0653]
The study found that P-4 promoted the oxidation of SO2 by generating O-3, while H3PO4 inhibited the desulfurization efficiency. In the liquid phase desulfurization process, the oxidation reaction of SO2 by O-3 was identified as the rate-determining step.
In this work, experimental and theoretical methods were used to investigate the catalytic effect of P-4 on SO2 oxidation in the liquid phase. Experimental results indicated that P-4 promoted SO2 oxidation by generating O-3. Meanwhile, the desulfurization efficiency was inhibited by H3PO4. Theoretical results indicated that the preferential adsorption of O-2 over P-4 was beneficial to the formation of O-3. Furthermore, the free O atom was a key role in forming O-3 and P4O due to the oxidation ability of O-3 and P4O for SO2. In the liquid phase desulfurization process, O-2 and SO2 were firstly dissolved into the liquid phase. Then, O-3 and P4O were generated from the interaction of O-2 and P-4. Next, SO2 moved close to O-3 and was oxidized into SO3 without H3PO4. Finally, SO3 was hydrated into H2SO4 with H3PO4. The oxidation of SO2 by O-3 without H3PO4 was the rate-determining step in the desulfurization process. H3PO4 slightly promoted the hydration reaction of SO3 but inhibited the oxidation of SO2. In general, the formation of H(3)PO(4 )consumed P-4 and led to the decreasing desulfurization efficiency.
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