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Behavior of bimetallic Pd-Cr/Al_2O_3 and Pd-Cr/(Ce, Zr)O_x/Al_2O_3 catalysts for CO and NO elimination

机译:双金属Pd-Cr / Al_2O_3和Pd-Cr /(Ce,Zr)O_x / Al_2O_3催化剂去除CO和NO的行为

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摘要

A series of Pd-Cr bimetallic catalysts suppoted on a (Ce, Zr)O_x/Al_2O_3 mixed support of Al_2O_3 alone have been characterized using a combination of X-ray diffraction,electron paramagnetic resonance, and Raman spectroscopy and employing in situ diffuse reflectance intra-red Fourier transform and X-ray near-edge structure spectroscopy to analyze the redox and chemical processes taking place during the course of the CO+NO+O_2 reaction. The catalytic behavior of these bimetallic systems was strongly affected by the nature of the support. In the case of the alumina support, evidence for interactions between Pd and Cr was observed in the calcined state. under reaction conditions formation of a mixed oxide phase containing Pd(I) and Cr(III) appears to be responsible for the improvement in CO oxidation and for the detrimental effect in the NO reduction process with respect to a monometallic, Pd reference system. In the case of the (Ce, Zr)O_x/Al_2O_3 mixed support, the addition of Cr was less influential in terms of catalytic activity. Results for the latter are rationalized mainly on the basis of the absence of interaction between the metal components in the calcined state and the presence of surface entities containing Cr alone when metallic-like Pd particles are formed during the course of reaction.
机译:利用X射线衍射,电子顺磁共振和拉曼光谱技术结合原位漫反射光谱法表征了单独沉积在Al_2O_3的(Ce,Zr)O_x / Al_2O_3混合载体上的一系列Pd-Cr双金属催化剂-红色傅里叶变换和X射线近边缘结构光谱分析了CO + NO + O_2反应过程中发生的氧化还原和化学过程。这些双金属体系的催化行为受到载体性质的强烈影响。在氧化铝载体的情况下,在煅烧状态下观察到Pd和Cr之间相互作用的证据。在反应条件下,含有Pd(I)和Cr(III)的混合氧化物相的形成似乎是对CO氧化的改善和NO还原过程中相对于单金属Pd参考体系的不利影响的原因。在(Ce,Zr)O_x / Al_2O_3混合载体的情况下,Cr的添加对催化活性的影响较小。后者的结果主要是基于在煅烧状态下金属组分之间不存在相互作用以及在反应过程中形成金属状Pd颗粒时仅包含Cr的表面实体的存在而合理化的。

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