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Precursor Effects on Catalytic Behaviors of Copper–Manganese–Cerium Ternary Oxides Pellets for Low-Temperature CO Oxidation
Catalysis Letters ( IF 2.3 ) Pub Date : 2019-10-15 , DOI: 10.1007/s10562-019-02992-4
Yafei Guo , Jin Lin , Jian Sun , Jubing Zhang , Changhai Li , Shouxiang Lu

Abstract Catalytic oxidation of CO into CO 2 using copper–manganese–cerium (Cu–Mn–Ce) ternary oxides pellets represents a promising strategy for CO abatement. In this work, Cu–Mn–Ce ternary oxides catalyst pellets were prepared with different precursors by combining the wet-mixing-kneading and extrusion-spheronization methods. Physicochemical properties of the catalyst pellets were characterized by N 2 adsorption–desorption, X-ray diffraction, scanning electron microscopy, X-ray energy dispersive spectrometry, transmission electron microscopy, X-ray photoelectron spectroscopy and H 2 -temperature programmed reduction. CO oxidation performance of the catalyst pellets were investigated in 0.5%CO, 2.0%H 2 O and balanced air using a fixed-bed reactor. Effects of granulation and precursor on the structure–activity relationships of the catalyst pellets were studied. The granulation process will adversely affect the CO oxidation performance of the as-prepared Cu–Mn–Ce ternary oxides catalysts. The catalyst pellet derived from nitrate precursors (CuMnCe-N) exhibits excellent CO oxidation activity (T 50 = 115 °C), good time-on-stream stability (retains about 97% conversion after 85 min of reaction tested) and superior kinetic performance (Ea = 40.32 kJ/mol). The excellent CO oxidation performance is associated with the formed Cu–Ce–O solid solution, enhanced reducibility and dual synergistic effects. Besides, the desired catalyst pellet possesses good mechanical properties with a high mechanical strength of 14.70 MPa and a low attrition rate of 9.46%. The results will provide important guidance for designing efficient catalysts for CO oxidation. Graphic Abstract

中文翻译:

前驱体对铜-锰-铈三元氧化物球团低温 CO 氧化催化行为的影响

摘要 使用铜-锰-铈 (Cu-Mn-Ce) 三元氧化物球团将 CO 催化氧化为 CO 2 是一种很有前景的 CO 减排策略。在这项工作中,通过结合湿混-捏合和挤出-滚圆方法,用不同的前驱体制备了 Cu-Mn-Ce 三元氧化物催化剂颗粒。通过N 2 吸附-解吸、X 射线衍射、扫描电子显微镜、X 射线能量色散光谱、透射电子显微镜、X 射线光电子能谱和H 2 程序升温还原表征了催化剂颗粒的物理化学性质。使用固定床反应器在 0.5%CO、2.0%H 2 O 和平衡空气中研究催化剂颗粒的 CO 氧化性能。研究了造粒和前体对催化剂颗粒结构-活性关系的影响。造粒过程将对所制备的 Cu-Mn-Ce 三元氧化物催化剂的 CO 氧化性能产生不利影响。源自硝酸盐前体 (CuMnCe-N) 的催化剂颗粒表现出优异的 CO 氧化活性 (T 50 = 115 °C)、良好的运行时间稳定性(测试反应 85 分钟后保持约 97% 的转化率)和优异的动力学性能(Ea = 40.32 kJ/mol)。优异的 CO 氧化性能与形成的 Cu-Ce-O 固溶体、增强的还原性和双重协同效应有关。此外,所需的催化剂颗粒具有良好的机械性能,具有 14.70 MPa 的高机械强度和 9.46% 的低磨损率。研究结果将为设计用于 CO 氧化的高效催化剂提供重要指导。图形摘要
更新日期:2019-10-15
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