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Novel Mn–Ce bi-oxides loaded on 3D monolithic nickel foam for low-temperature NH3-SCR de-NOx: Preparation optimization and reaction mechanism
Journal of Rare Earths ( IF 5.2 ) Pub Date : 2020-12-29 , DOI: 10.1016/j.jre.2020.12.015
Shuquan Ni , Xiaolong Tang , Honghong Yi , Fengyu Gao , Chengzhi Wang , Yiran Shi , Runcao Zhang , Wenjuan Zhu

This study explored the superior citrate method (CM) to synthesize Mn–Ce bi-oxides on 3D monolithic Ni-foam (NF) catalysts for the selective catalytic reduction of NO by NH3 (NH3-SCR). The 17 wt% Mn(7)Ce(3)Ox/NF (CM-17) catalyst shows the NOx conversion of 98.7% at 175 °C and 90% in the presence of 10 vol% H2O. It is revealed that the combination of surface-active oxygen (formed by high-level oxygen vacancies) and strongly oxidized Mn4+ species promots the Fast-SCR reactions, in which Mn4+ species play a leading role in NH3-SCR reaction, and the unsaturated Ni atoms and also Ce3+ species promote electron exchange and thus improve the redox performance. The coexistence mechanisms of Fast-SCR reactions and E-R pathways are observed over Mn-CeOx/NF catalyst, which may be promoted by the Brønsted sites at low temperature. In addition, the heat resistance, stability, 3D monolithic porous structure and excellent physical properties of foam nickel provide a unique growth substrates for catalysts preparation and reaction sites for NOx purification. Therefore, industrial application of Mn–Ce bi-oxides loaded on 3D monolithic is proposed to be achieved through reasonable preparation methods.



中文翻译:

新型 Mn-Ce 二氧化物负载 3D 整体式镍泡沫用于低温 NH3-SCR 脱硝:制备优化和反应机理

本研究探索了在 3D 整体式泡沫镍 (NF) 催化剂上合成 Mn-Ce 二氧化物的优越柠檬酸盐法 (CM),用于 NH 3 (NH 3 -SCR) 选择性催化还原 NO。17 wt% Mn(7)Ce(3)O x /NF (CM-17) 催化剂在 175 °C 下的 NO x转化率为 98.7%,在 10 vol% H 2 O存在下为 90%。揭示了表面活性氧(由高水平氧空位形成)和强氧化的Mn 4+物质的结合促进了Fast-SCR反应,其中Mn 4+物质在NH 3 -SCR反应中起主导作用,并且不饱和Ni原子和Ce 3+物种促进电子交换,从而提高氧化还原性能。在 Mn-CeO x /NF 催化剂上观察到 Fast-SCR 反应和 ER 途径的共存机制,这可能由低温下的 Brønsted 位点促进。此外,泡沫镍的耐热性、稳定性、3D 整体多孔结构和优异的物理性能为催化剂制备和 NO x净化的反应位点提供了独特的生长基质。因此,建议通过合理的制备方法实现负载在 3D 单片上的 Mn-Ce 二氧化物的工业应用。

更新日期:2020-12-29
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