H/D exchange studies of methane activation mechanisms in heterogeneous catalysis

D. Zakharov
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Abstract

The development of technologies for the efficient conversion of methane and other light hydrocarbons is becoming vital to the chemical industry. The main technologies for methane conversion are based on solid and liquid catalysts such as metals, oxides and oxide-supported metals. Methane is a highly stable molecule, and the analysis of the catalytic activity of materials with respect to the C-H bond cleavage in methane is of paramount importance for the development of novel methane conversion catalysts. One of the most promising methods for studying methane activation over a catalyst is H/D isotope exchange between the gas and condensed phases. The method provides reliable in situ information on the cleavage of chemical bonds in molecules and allows researchers to elucidate the elementary steps of catalytic methane activation and the stable intermediates involved in the activation process. This paper focuses on the critical analysis of H/D isotope exchange studies of the methane activation mechanism over various metals, oxides, composites, and other catalysts, from the earlier studies to the recent advances in the field. The existing theoretical and experimental approaches to study the H/D exchange between methane and a catalyst are discussed in the paper. A critical analysis of the structure-composition-catalytic activity relationships of the catalysts with respect to methane activation is provided.
多相催化中甲烷活化机理的H/D交换研究
开发有效转化甲烷和其他轻烃的技术对化学工业来说正变得至关重要。甲烷转化的主要技术是基于固体和液体催化剂,如金属、氧化物和氧化物负载金属。甲烷是一种高度稳定的分子,分析材料对甲烷中C-H键裂解的催化活性对开发新型甲烷转化催化剂具有重要意义。研究甲烷在催化剂上活化的最有前途的方法之一是气相和凝聚相之间的H/D同位素交换。该方法提供了分子中化学键断裂的可靠的原位信息,使研究人员能够阐明催化甲烷活化的基本步骤和参与活化过程的稳定中间体。本文重点分析了甲烷在各种金属、氧化物、复合材料和其他催化剂上活化机理的H/D同位素交换研究,从早期的研究到该领域的最新进展。本文讨论了目前研究甲烷与催化剂H/D交换的理论和实验方法。对催化剂的结构-组成-催化活性与甲烷活化的关系进行了批判性分析。
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