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Steady-state and unsteady-state kinetic approaches for studying reactions over three-way natural gas vehicle catalysts

机译:用于研究三元天然气汽车催化剂反应的稳态和非稳态动力学方法

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摘要

Kinetics has been proven to be a powerful method to probe catalytic surfaces under reaction conditions in order to elucidate, at molecular level, complex chemical processes Numerous techniques and methodologies have been already implemented (surface science approaches, TAP, SSITKA...) running in very different pressure ranges (pressure gap) which led to controversial statements regarding suggested mechanism schemes, especially for DeNO_x reactions. Two typical reactions taking place over NGV catalysts have been selected to illustrate which information can be tackled from kinetic measurements. Both reactions occur in different temperature ranges and are sensitive to the structure of the catalyst, to the surface composition of bimetallic particles, with possible surface enrichments, and to the participation of the support. Hence, it will be tentatively demonstrated that kinetic combined with spectroscopic or theoretical methods can be appropriate to establish relevant correlations between kinetic parameters and the topology of the catalyst surface.
机译:动力学已被证明是一种在反应条件下探测催化表面的强大方法,以便在分子水平上阐明复杂的化学过程,现已应用了许多技术和方法(表面科学方法,TAP,SSITKA ...)非常不同的压力范围(压力差)导致有关建议的机理方案,特别是对于DeNO_x反应的争议性陈述。选择了在NGV催化剂上发生的两个典型反应,以说明可以从动力学测量中解决的信息。两种反应均在不同的温度范围内发生,并且对催化剂的结构,双金属颗粒的表面组成,可能的表面富集以及载体的参与均敏感。因此,将初步证明动力学与光谱学或理论方法相结合可以适当地建立动力学参数与催化剂表面拓扑之间的相关关系。

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