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Ce-TiO 在 SO 存在下的选择性催化还原(SCR)性能的温度敏感性。

Temperature sensitivity of the selective catalytic reduction (SCR) performance of Ce-TiO in the presence of SO.

机构信息

Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing, 210096, Jiangsu, PR China.

Engineering Laboratory of Energy System Process Conversion & Emission Control Technology of Jiangsu Province, School of Energy and Mechanical Engineering, Nanjing Normal University, Nanjing, 210042, PR China.

出版信息

Chemosphere. 2020 Mar;243:125419. doi: 10.1016/j.chemosphere.2019.125419. Epub 2019 Nov 22.

Abstract

Cerium titanate catalyst (Ce-TiO) is competitive as a substitute for the commercial SCR (selective catalytic reduction) catalysts VO-WO/TiO due to its high SCR activity and excellent redox performance. The reaction mechanisms of Ce-TiO at 180 °C, 240 °C, and 300 °C in the presence of SO were systematically studied regarding the evolution of the SCR activity, quantitative analysis of sulfate compounds, and comprehensive identification of the fresh and poisoned catalysts. The results demonstrated that NO conversion at 180 °C in the presence of SO is highly sensitive to the formation of cerium sulfates/sulfites, limiting the reactivity of NH adsorbed on SO Brønsted acid sites and inhibiting the E-R reaction pathway. At 240 °C, the degradation of NO conversion was commenced by the cumulative influence of cerium sulfates/sulfites. With the increase of the reaction temperature to 300 °C, the NO conversion is gradually immune to the formation of cerium sulfates in spite of the great amount of cerium sulfates deposited on the deeper interior of CeO. The high SCR activity of the Ce-TiO catalyst in the presence of SO at a higher reaction temperature might be ascribed to the synergistic catalysis between surface cerium sulfates and bulk CeO, where surface cerium sulfates act as acid sites for the adsorption of NH and the bulk CeO acts as the redox sites. The reaction mechanisms of the Ce-TiO catalyst in the presence of SO at different temperatures are proposed as the two reaction routes.

摘要

铈钛催化剂(Ce-TiO)作为商业 SCR(选择性催化还原)催化剂 VO-WO/TiO 的替代品具有竞争力,因为它具有高的 SCR 活性和优异的氧化还原性能。在 SO 存在下,系统研究了 Ce-TiO 在 180°C、240°C 和 300°C 时的反应机制,包括 SCR 活性的演变、硫酸盐化合物的定量分析以及新鲜和中毒催化剂的综合鉴定。结果表明,180°C 时 SO 存在下的 NO 转化率对硫酸铈/亚硫酸铈的形成非常敏感,限制了 NH 在 SO Brønsted 酸位上的吸附反应性,并抑制了 E-R 反应途径。在 240°C 时,NO 转化率的降解是由硫酸铈/亚硫酸铈的累积影响开始的。随着反应温度升高至 300°C,尽管大量的硫酸铈沉积在 CeO 的更深层内部,但 NO 转化率逐渐不受硫酸铈形成的影响。在较高的反应温度下,Ce-TiO 催化剂在 SO 存在下具有较高的 SCR 活性,这可能归因于表面硫酸铈和体相 CeO 之间的协同催化作用,其中表面硫酸铈作为 NH 的吸附酸位,而体相 CeO 作为氧化还原位。提出了在不同温度下 SO 存在下 Ce-TiO 催化剂的反应机制,包括两条反应途径。

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