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主要通过XPS表征、热力学计算以及一系列设计的评价实验等方法,对硫化CoMo/Al2O3催化剂上H2同时催化还原SO2和NO反应的活性相、吸附活性位以及反应机理进行了研究。结果表明,金属硫化物相是SO2和NO转化的主要活性相,并与载体Al2O3共同承担H2S转化为单质硫的作用。此外,反应过程中产生的晶格空位也对NO转化起着重要作用。催化剂表面的阴离子空位是SO2和NO共同的吸附活性位,SO2对NO的吸附有抑制作用,而催化剂表面的L碱位也是SO2的吸附活性位,NO可促进SO2的氧化吸附。最后,本文从反应分子的吸附与活化、NO的转化及晶格硫的流失、SO2还原到H2S、H2S的转化、晶格硫的补充等5个方面提出了反应机理。
The active sites, the active sites for adsorption and the reaction mechanism of simultaneous H2-catalyzed reduction of SO2 and NO on sulfided CoMo / Al2O3 catalysts were investigated by means of XPS characterization, thermodynamic calculation and a series of evaluation experiments. The results show that the metal sulphide phase is the main active phase for the conversion of SO2 and NO, and co-undertakes the conversion of H2S to elemental sulfur with the carrier Al2O3. In addition, lattice vacancies generated during the reaction also play an important role in NO conversion. The anion vacancies on the catalyst surface are the common adsorption active sites for SO2 and NO. SO2 can inhibit the adsorption of NO, while the L base on the catalyst surface is also the active site for SO2 adsorption. NO promotes the oxidation and adsorption of SO2. Finally, the reaction mechanism is proposed in this paper from five aspects: adsorption and activation of reaction molecules, conversion of NO and loss of lattice sulfur, reduction of SO2 to H2S, conversion of H2S and addition of lattice sulfur.