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首页> 外文期刊>Catalysis science & technology >A new insight into SO2 low-temperature catalytic oxidation in porous carbon materials: non-dissociated O-2 molecule as oxidant
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A new insight into SO2 low-temperature catalytic oxidation in porous carbon materials: non-dissociated O-2 molecule as oxidant

机译：一个新的见解二氧化硫低温催化氧化多孔碳材料:non-dissociated 0 2分子作为氧化剂

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摘要

SO2 oxidation is the rate-determining step during the process of low-temperature SO2 conversion to high-value H2SO4 in porous carbon materials. Non-dissociated O-2 molecules and chemisorbed O atoms from O-2 dissociation are possible oxidants for SO2 oxidation. While the pathways of oxidation reactions in which chemisorbed O atoms participate have been previously studied via density functional theory calculation, the possible SO2 oxidation pathways by non-dissociated O-2 remain to be investigated. Inspired by the mechanism in which a non-dissociated O-2 molecule oxidizes other molecules such as CO and NO, we elucidate the detailed pathways for SO2 oxidation by non-dissociated O-2 using density functional theory calculation assisted by SO2 removal experiment validation. Computational results show that non-dissociated O-2 can be activated at the active sites of porous carbon, generating a C-O-O structure. By low-barrier O transfer processes, the formed C-O-O structure can directly oxidize gaseous SO2 to SO3 without the need of the SO2 chemisorption process. Transient response experiments further validate that the oxidant for SO2 conversion to SO3 in porous carbon materials is non-dissociated O-2. This work reveals the role of non-dissociated O-2 in directly oxidizing non-chemisorbed SO2 to SO3 at low temperature, providing a new understanding for SO2 conversion to SO3 in porous carbon materials.
机译：二氧化硫氧化的速率决定步骤低温二氧化硫转化的过程高价值的硫酸在多孔碳材料。Non-dissociated 0 2分子和化学吸附O原子从0 2分离是可能的氧化剂对二氧化硫氧化。氧化反应的化学吸附O原子参加之前通过学习密度泛函理论计算,可能的二氧化硫氧化途径non-dissociated 0 2仍有待调查。受的机制non-dissociated 0 2分子氧化分子如公司不,我们阐明了详细的二氧化硫氧化的途径使用密度泛函non-dissociated坐坐理论计算得到二氧化硫去除实验验证。, non-dissociated 0 2可以激活的活跃的多孔碳,生成C-O-O结构。可以直接氧化形成C-O-O结构气态二氧化硫SO2的SO3而不需要化学吸收作用过程。实验进一步验证的氧化剂二氧化硫转化SO3的多孔碳材料是non-dissociated坐坐。在直接氧化作用non-dissociated坐坐non-chemisorbed二氧化硫在低温SO3,为二氧化硫转化提供了一个新的理解SO3的多孔碳材料。

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