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The effect of trivalent framework heteroatoms in Cu-CHA on the Selective Catalytic Reduction of NO
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2021-08-25 , DOI: 10.1016/j.apcata.2021.118326
Patrick Tomkins 1 , Bernd Marler 2 , Robert McGuire 3 , Ulrich Müller 3 , Mathias Feyen 3 , Andrei-Nicolae Parvulescu 3 , Weiping Zhang 4 , Toshiyuki Yokoi 5 , Feng-Shou Xiao 6 , Hermann Gies 2 , Ute Kolb 7 , Haishuang Zhao 7 , Pieterjan Valvekens 1 , Trees De Baerdemaeker 1 , Dirk De Vos 1
Affiliation  

The effect of the trivalent framework atoms (Si4+/M3+ = 13-105) in Cu exchanged CHA-type zeolites was investigated for the selective catalytic reduction of NO with NH3. While the increased hydrophobicity of B-CHA compared to Al-CHA could make it a good candidate for low temperature SCR, the material was too unstable under reaction conditions and the exchanged Cu2+ did not remain isolated. Consequently a lower activity and selectivity than for Al-CHA were observed. Ga-CHA on the other hand showed a similar Cu2+ speciation as Al-CHA at similar Si4+/M3+ ratios. The difference in catalytic activity was remarkably small. While Ga-CHA was less stable upon hydrothermal aging, this was markedly improved by increasing the Si/Ga ratio and by inserting the Cu2+ during the synthesis of the zeolite. Remarkably, the Cu-loaded Ga-CHA catalysts demonstrated a consistently lower selectivity to N2O by-product formation compared to Al-CHA because of a lower tendency for NO oxidation.



中文翻译:

Cu-CHA中三价骨架杂原子对NO选择性催化还原的影响

研究了Cu 交换 CHA 型沸石中三价骨架原子 (Si 4+ /M 3+ = 13-105) 对用 NH 3选择性催化还原 NO 的影响。虽然与 Al-CHA 相比,B-CHA 增加的疏水性使其成为低温 SCR 的良好候选者,但该材料在反应条件下太不稳定,并且交换的 Cu 2+不会保持分离。因此,观察到比 Al-CHA 更低的活性和选择性。另一方面,Ga-CHA在相似的 Si 4+ /M 3+ 下表现出与Al-CHA相似的 Cu 2+形态比率。催化活性的差异非常小。虽然Ga-CHA 在水热老化时稳定性较差,但通过增加Si/Ga 比和在沸石合成过程中插入Cu 2+ 可以显着改善这一点。值得注意的是,与 Al-CHA 相比,负载 Cu 的 Ga-CHA 催化剂对 N 2 O 副产物形成的选择性始终较低,因为 NO 氧化的趋势较低。

更新日期:2021-09-17
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