Abstract

Temporal Analysis of Products (TAP) investigation on Natural Gas-fueled Vehicle (NGV) catalysts provides information related to the nature of reaction steps involved over noble metals and at the metal-support interface. The determination of accurate kinetic parameters for methane adsorption from single pulse experiments and subsequent investigation of sequential surface reactions from alternative CH4/O2 pulse experiments is the first step toward the establishment of relevant structure/activity relationships which can highlight the importance of the metal/support interface on freshly-prepared and aged single palladium based catalysts.

Highlights

  • AND SCIENTIFIC BACKGROUNDTemporal Analysis of Products (TAP) reactors allow qualitative and quantitative characterization of the kinetics of elementary steps such as adsorption, surface reactions, and diffusion processes on a wide variety of catalysts

  • This paper offers a quantitative view of the real impact of the metal/support interface based on a precise determination of kinetic constants from modeling single pulse experiments (SP) experiments taking into account the peculiar porous properties of the materials

  • The initial fast process is not accompanied with a parallel CO formation that underlines the predominant CH4 decomposition to gaseous H2 and chemisorbed carbidic species (Cads) on Pd active centers described in Scheme 1

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Summary

Introduction

AND SCIENTIFIC BACKGROUNDTemporal Analysis of Products (TAP) reactors allow qualitative and quantitative characterization of the kinetics of elementary steps such as adsorption, surface reactions, and diffusion processes on a wide variety of catalysts. The determination of accurate kinetic parameters for methane adsorption from single pulse experiments and subsequent investigation of sequential surface reactions from alternative CH4/O2 pulse experiments is the first step toward the establishment of relevant structure/activity relationships which can highlight the importance of the metal/support interface on freshly-prepared and aged single palladium based catalysts.

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