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Ce/TiO催化剂用于NH₃选择性催化还原NO的硫化作用:机理与动力学研究

Sulfation effect of Ce/TiO catalyst for the selective catalytic reduction of NO with NH: mechanism and kinetic studies.

作者信息

Zhang Wenjie, Liu Guofu, Jiang Jie, Tan Yuchen, Wang Qi, Gong Chenghong, Shen Dekui, Wu Chunfei

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

RSC Adv. 2019 Oct 9;9(55):32110-32120. doi: 10.1039/c9ra06985b. eCollection 2019 Oct 7.

Abstract

Ceria-based catalysts are competitive substitutes for the commercial SCR catalysts due to their high SCR activity and excellent redox performance. For a better understanding of the SO poisoning mechanism over ceria-based catalysts, the sulfation effect of the Ce/TiO catalyst on the SCR activity over a wide reaction temperature range was systematically studied comprehensive characterizations, DRIFT studies and kinetic studies. The results demonstrated that the NO conversion at 150 °C is significantly inhibited by the formation of cerium sulfites/sulfates due to the inhibited redox properties and excessive adsorption of NH, which restrict the dissociation of NH to NH, resulting in a much lower reaction rate of E-R reaction over the sulfated Ce/TiO catalyst. With the increase in the reaction temperature, the reaction rate of the E-R reaction significantly increased due to the improved redox properties and weakened adsorption of NH. Moreover, the rate of the C-O reaction over the sulfated Ce/TiO catalysts is obviously lower than that of the fresh Ce/TiO catalyst. The promotion of NO conversion over the sulfated catalyst at 330 °C is attributed to both the increase in the reaction rate of E-R reaction and the inhibition of the C-O reaction.

摘要

基于铈的催化剂因其高选择性催化还原(SCR)活性和优异的氧化还原性能,是商业SCR催化剂的有竞争力的替代品。为了更好地理解基于铈的催化剂上的SO中毒机理,通过综合表征、漫反射红外傅里叶变换光谱(DRIFT)研究和动力学研究,系统地研究了Ce/TiO催化剂的硫酸化作用对宽反应温度范围内SCR活性的影响。结果表明,在150°C时,由于铈亚硫酸盐/硫酸盐的形成抑制了氧化还原性能以及NH的过度吸附,NO转化率受到显著抑制,这限制了NH解离为NH,导致硫酸化Ce/TiO催化剂上E-R反应的反应速率低得多。随着反应温度的升高,由于氧化还原性能的改善和NH吸附的减弱,E-R反应的反应速率显著增加。此外,硫酸化Ce/TiO催化剂上C-O反应的速率明显低于新鲜Ce/TiO催化剂。在330°C时硫酸化催化剂上NO转化率的提高归因于E-R反应速率的增加和C-O反应的抑制。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9717/9072935/8425c56f8a1d/c9ra06985b-f1.jpg

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