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深入了解 Cu-SSZ-13 催化剂中 Cu 离子和 CuO 物种对 NH3 选择性催化还原 NO 的影响。

Insight into the effects of Cu ions and CuO species in Cu-SSZ-13 catalysts for selective catalytic reduction of NO by NH.

机构信息

College of Environmental Science and Engineering, Dalian Maritime University, Dalian 116026, China.

College of Environmental Science and Engineering, Dalian Maritime University, Dalian 116026, China.

出版信息

J Colloid Interface Sci. 2022 Sep 15;622:1-10. doi: 10.1016/j.jcis.2022.04.110. Epub 2022 Apr 25.

Abstract

Different Cu precursors were adopted to adjust the isolated Cu ions and CuO species in the Cu-SSZ-13 catalysts. The Cu ions were mainly located at eight-member rings in the catalysts with the Cu precursors of Cu(NO) (Fresh-I) and CuSO (Fresh-II), while that located at six-member rings in the catalysts with the Cu precursors of CuCl (Fresh-III) and Cu(CHCOO) (Fresh-IV). All catalysts showed>90% of NO conversion and 100% of N selectivity at 200-680 °C. Fresh-I and Fresh-II catalysts showed an unexpected increase of the high-temperature activity after hydrothermal treatment. The characterizations revealed that the hydrothermal treatment promoted the production of CuO species, which accelerated the adsorption of NO species to enhance the high-temperature SCR activity. Moreover, the SCR reaction pathway changed from Langmuir-Hinshelwood to Eley-Rideal mechanisms for the Fresh-II catalyst after the hydrothermal treatment, which was verified by in situ DRIFTS.

摘要

采用不同的 Cu 前驱体来调整 Cu-SSZ-13 催化剂中孤立的 Cu 离子和 CuO 物种。Cu 离子主要位于催化剂的八元环中,Cu(NO)(Fresh-I)和 CuSO(Fresh-II)为前驱体;而 CuCl(Fresh-III)和 Cu(CHCOO)(Fresh-IV)为前驱体时,Cu 离子位于六元环中。所有催化剂在 200-680°C 时均表现出>90%的 NO 转化率和 100%的 N 选择性。经水热处理后,Fresh-I 和 Fresh-II 催化剂的高温活性出人意料地增加。表征结果表明,水热处理促进了 CuO 物种的生成,从而加速了 NO 物种的吸附,提高了高温 SCR 活性。此外,水热处理后,Fresh-II 催化剂的 SCR 反应途径从 Langmuir-Hinshelwood 机制转变为 Eley-Rideal 机制,这通过原位 DRIFTS 得到了验证。

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