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Light alkane oxidation over well-defined active sites in metal-organic framework materials

机译:金属有机框架材料中定义明确的活性位点上的轻烷烃氧化

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摘要

The single-step conversion of light alkanes to chemical/energy carriers that can be readily transported over long distances is a critical component in the effort to effectively valorize vast reserves of shale gas resources in the United States and around the world. Catalyst materials traditionally investigated for such applications - although exhibiting promising alkane oxidation performance - typically display a broad distribution of active site speciation within individual formulations, making it challenging to develop generalizable principles guiding the rational design of highly active and selective catalysts. Metal-organic framework materials (MOFs) enable a high level of definition and uniformity in active site structure, as well as a multitude of alternatives in terms of active site coordination environment, thereby potentially enabling a more rigorous understanding of the relationship between structure and catalytic function. This review provides an overview of key examples of MOF-catalyzed C1-C3 alkane oxidation that have been reported in the literature, with an emphasis on active site characterization, reaction mechanisms, and proposed structure-function relationships. Also presented and discussed are critical knowledge gaps and future prospects for this burgeoning (but still nascent) area of research.
机译:可以在长距离上容易运输的轻烷烃到化学/能源载体的单步转换是有效地在美国和世界各地有效地重视大量页岩气资源的关键组成部分。传统上研究了此类应用的催化剂材料(尽管表现出有希望的烷烃氧化性能)通常在单个配方中显示出广泛的现场物种形成的分布,这使得开发具有高度活跃和选择性催化剂的合理设计的可普遍原则的挑战。金属有机框架材料(MOF)可以在主动地点结构中具有高水平的定义和均匀性,以及在主动站点协调环境方面的多种替代方案,从而有可能对结构与催化之间的关系有更严格的了解功能。这篇综述概述了文献中已经报道的MOF催化的C1-C3烷烃氧化,重点是主动位点表征,反应机制和提出的结构 - 功能关系。还介绍和讨论的是这个新兴(但仍然新生)的研究领域的关键知识差距和未来前景。

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