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Durable ruthenium oxide/ceria catalyst with ultralarge mesopores for low-temperature CO oxidation
Journal of Catalysis ( IF 6.5 ) Pub Date : 2020-01-03 , DOI: 10.1016/j.jcat.2019.12.021
Albert A. Voskanyan , Chi-Kin Jenkin Tsui , Kwong-Yu Chan

With more stringent CO emission limits, the development of efficient and durable catalysts for low-temperature (<200 °C) CO oxidation is crucial for the automotive industry. Here we report significant improvement in catalytic activity by incorporation of RuO2 into the CeO2 lattice. The Ru0.15Ce0.85O2-y demonstrates the highest catalytic activity with T100 value of 165 °C (rCO = 3.65 × 10−5 mol gcat−1 s−1), corresponding to activation energy of 49.8 kJ mol−1. The TOF of Ru0.15Ce0.85O2-y (48.6 × 10−3 s−1) is approximately 20 times higher than that of Ru0.015Ce0.975O2-y (2.48 × 10−3 s−1) and Ru0.3Ce0.7O2-y (2.72 × 10−3 s−1) catalysts at 160 °C. The catalyst remained stable after 70 h continuous operation under high GHSV (150000 ml g−1 h−1) without any noticeable compositional and structural changes. The necessity of using CO-TPR instead of commonly used H2-TPR analysis is presented to assess the surface reducibility of the catalysts for CO oxidation reaction. Based on the structural characterizations combined with kinetic studies, we find the catalyst surface reducibility by CO determines the activity in CO oxidation.



中文翻译:

具有超大介孔的耐用氧化钌/二氧化铈催化剂,用于低温CO氧化

随着更严格的CO排放限制,开发用于低温(<200°C)CO氧化的高效耐用催化剂对于汽车行业至关重要。在这里,我们报道通过将RuO 2掺入CeO 2晶格中,催化活性得到了显着改善。在Ru 0.150.85 ö 2-Y表明的最高的催化活性和T 100的值165°C(R CO  = 3.65×10 -5摩尔克-1小号-1),对应于49.8千焦摩尔的活化能- 1。Ru 0.15 Ce 0.85 O的TOF2-y(48.6×10 -3 s -1)比Ru 0.015 Ce 0.975 O 2-y(2.48×10 -3 s -1)和Ru 0.3 Ce 0.7 O 2-y(2.72 )高约20倍× 160 -3 s -1)催化剂在160°C下。在高GHSV(150000 ml g -1 h -1)下连续运行70 h后,催化剂保持稳定,而没有任何明显的组成和结构变化。使用CO-TPR代替常用的H 2的必要性提出了-TPR分析以评估用于CO氧化反应的催化剂的表面还原性。基于结构特征并结合动力学研究,我们发现通过CO还原催化剂的表面活性决定了CO氧化的活性。

更新日期:2020-01-04
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