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Optimization of N2O decomposition activity of CuO–CeO2 mixed oxides by means of synthesis procedure and alkali (Cs) promotion
Catalysis Science & Technology ( IF 5 ) Pub Date : 2018-03-29 00:00:00 , DOI: 10.1039/c8cy00316e
Maria Lykaki 1, 2, 3, 4 , Eleni Papista 4, 5, 6, 7 , Sónia A. C. Carabineiro 8, 9, 10, 11, 12 , Pedro B. Tavares 13, 14, 15, 16, 17 , Michalis Konsolakis 1, 2, 3, 4
Affiliation  

The fine-tuning of local surface chemistry of CuO–CeO2 mixed oxides by means of synthesis procedure and alkali promotion towards the rational design of highly active catalysts is investigated. In particular, the impact of alkali (Cs) promotion on the N2O decomposition activity (deN2O process) of CuO–ceria mixed oxides, pre-optimized through the preparation procedure (co-precipitation among different synthesis routes), is explored. It was found that the co-optimization of the synthesis procedure (co-precipitation) and alkali loading (1.0 at Cs per nm2) can boost the decomposition of N2O and resistance to O2 inhibition, offering a half-conversion temperature (T50) ca. 200 °C lower, when compared to a reference CuO–CeO2 sample. A complementary characterization study involving surface area determination (BET method), pore size distribution (BJH method), X-ray diffraction (XRD), H2 temperature-programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS) was undertaken to gain insight into structure–property relationships. The results revealed that the superiority of Cs-doped samples can be mainly attributed to the electronic effect of the alkali promoter towards the stabilization of partially reduced Cu+/Ce3+ pairs, which play a key role in the deN2O process following a redox-type mechanism.

中文翻译:

合成步骤和碱(Cs)促进法 优化CuO–CeO 2混合氧化物 的N 2 O分解活性

研究了CuO–CeO 2混合氧化物的局部表面化学的微调,该过程通过合成程序和碱促进朝着合理设计高活性催化剂的方向发展。尤其是,探讨了碱促进(Cs)对通过制备方法(不同合成路线之间的共沉淀)预先优化的CuO-二氧化铈混合氧化物的N 2 O分解活性(deN 2 O工艺)的影响。 。发现合成工艺(共沉淀)和碱负荷(在Cs / nm 2下为1.0)的共同优化可以促进N 2 O的分解和抗O 2的抑制作用,从而提供半转化温度(Ť50与参考CuO–CeO 2样品相比,低200°C。补充表征研究,涉及表面积测定(BET法),孔径分布(BJH方法),X射线衍射(XRD),H 2程序升温还原(H 2 -TPR)和X射线光电子能谱(XPS)旨在深入了解结构与财产之间的关系。结果表明,掺杂Cs的样品的优越性主要归因于碱促进剂对部分还原的Cu + / Ce 3+对的稳定作用的电子效应,这在脱氮后的deN 2 O过程中起着关键作用。氧化还原型机制。
更新日期:2018-03-29
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