Synergy between hydrogen and ceria in Pt-catalyzed CO oxidation: An investigation on Pt–CeO2 catalysts synthesized by solution combustion

催化作用 近程 初湿浸渍 化学 无机化学 X射线光电子能谱 铂金 催化燃烧 选择性 核化学 一氧化碳 化学工程 有机化学 工程类
作者
F. Morfin,Thanh‐Son Nguyen,Jean‐Marc Rousset,L. Piccolo
出处
期刊:Applied Catalysis B-environmental [Elsevier]
卷期号:197: 2-13 被引量:85
标识
DOI:10.1016/j.apcatb.2016.01.056
摘要

Pt–CeO2 catalysts were prepared by solution combustion synthesis (SCS), a simple and fast one-pot method, using glycine or oxalyl dihydrazide (ODH) as the fuel and Pt chloride or nitrate as the metal precursor. The samples were characterized by ICP-OES, N2 volumetry, XRD, XPS, aberration-corrected (S)TEM, CO-DRIFTS and microRaman spectroscopy. The SCS catalysts were evaluated in CO oxidation and preferential oxidation (PROX) of CO in H2 excess, and compared to Pt/CeO2 and Pt/Al2O3 catalysts prepared by incipient wetness impregnation. The glycine fuel yields better results than ODH in terms of Pt dispersion and catalytic performance. The fresh Cl-containing catalysts consist of PtO nanoparticles poorly active in CO oxidation, while the catalysts synthesized from Pt nitrate contain highly active Ptδ+ (0 < δ < 2) species in interaction with ceria. Consistently, the most efficient catalyst for H2-free CO oxidation is the one synthesized from glycine and Pt nitrate. For PROX, the selectivity to CO2 is 100% at low temperature and decreases in a similar way for all the Pt–CeO2 catalysts above ca. 100 °C. With respect to H2-free conditions, the CO PROX activity of the Pt–CeO2 catalysts is considerably enhanced (activity multiplied by up to 60 at 110 °C), while the activity gain is comparatively minor for Pt/Al2O3. We conclude that hydrogen, by increasing the mobility of oxygen species at the surface of ceria, promotes the support-assisted pathway of CO oxidation.

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