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Effect of Copper Precursors on the Activity and Hydrothermal Stability of Cu<sup>II</sup>−SSZ−13 NH<sub>3</sub>−SCR Catalysts
mā: Meixin Wang, Zhaoliang Peng, Changming Zhang, Mengmeng Liu, Lina Han, Yaqin Hou, Zhanggen Huang, Jiancheng Wang, Weiren Bao, Liping Chang
Hōputu: | Article |
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I whakaputaina: | MDPI AG 2019-09-01 |
Whakaahuatanga
A series of Cu<sup>II</sup>−SSZ−13 catalysts are prepared by in-situ hydrothermal method using different copper precursors (Cu<sup>II</sup>(NO<sub>3</sub>)<sub>2</sub>, Cu<sup>II</sup>SO<sub>4</sub>, Cu<sup>II</sup>Cl<sub>2</sub>) for selective catalytic reduction of NO by NH<sub>3</sub> in a simulated diesel vehicle exhaust. The catalysts were characterized by X−ray diffraction (XRD), scanning electron microscope (SEM), X−ray photoelectron spectroscopy (XPS), N<sub>2</sub> adsorption-desorption, hydrogen-temperature-programmed reduction (H<sub>2</sub>−TPR), ammonia temperature-programmed desorption (NH<sub>3</sub>−TPD), and <sup>27</sup>Al and <sup>29</sup>Si solid state Nuclear Magnetic Resonance (NMR). The Cu<sup>II</sup>−SSZ−13 catalyst prepared by Cu<sup>II</sup>(NO<sub>3</sub>)<sub>2</sub> shows excellent catalytic activity and hydrothermal stability. The NO conversion of Cu<sup>II</sup>−SSZ−13 catalyst prepared by Cu<sup>II</sup>(NO<sub>3</sub>)<sub>2</sub> reaches 90% at 180 °C and can remain above 90% at a wide temperature range of 180−700 °C. After aging treatment at 800 °C for 20 h, the Cu<sup>II</sup>−SSZ−13 catalyst prepared by Cu<sup>II</sup>(NO<sub>3</sub>)<sub>2</sub> still exhibits above 90% NO conversion under a temperature range of 240−600 °C. The distribution of Cu species and the Si/Al ratios in the framework of the synthesized Cu<sup>II</sup>−SSZ−13 catalysts, which determine the catalytic activity and the hydrothermal stability of the catalysts, are dependent on the adsorption capacity of anions to the cation during the crystallization process due to the so called Hofmeister anion effects, the NO<sub>3</sub><sup>−</sup> ion has the strongest adsorption capacity among the three kinds of anions (NO<sub>3</sub><sup>−</sup>, Cl<sup>−</sup>, and SO<sub>4</sub><sup>2−</sup>), followed by Cl<sup>−</sup> and SO<sub>4</sub><sup>2−</sup> ions. Therefore, the Cu<sup>II</sup>−SSZ−13 catalyst prepared by Cu<sup>II</sup>(NO<sub>3</sub>)<sub>2</sub> possess the best catalytic ability and hydrothermal stability.