Single-site Zn+ on CuFe clusters for the selective oxidation of methane to methanol

天然气的主要成分甲烷(CH4)的有效价态在催化中仍然是一个重大的挑战。已知CH4可以通过自由基途径(脱氢)或表面稳定的M-CH3途径(去质子化)在两个不同的活性中心上被催化活化。该项目旨在通过设计和合成嵌入在omega沸石中的由单价锌离子中心和CuFe-oxo簇合物组成的多功能催化剂，将这两个过程结合起来。通过这种策略的应用，人们认为甲烷脱质子和脱氢都可以同时实现。以往的文献已经证实，omega沸石可以容纳高浓度的铜或铁活性物种，从而为转化甲烷提供了丰富的活性中心。将配备连续流动固定床反应装置来研究该反应，以抑制CH3OH的过氧化生成较少的不良产物。最终，本项目的目标是(1)开发高效和选择性的甲烷转化为CH3OH的催化剂，以及(2)更好地了解不同的活性中心如何促进甲烷的活化和影响该过程中的反应选择性。尽管与新冠肺炎大流行相关的困难仍在继续，但将采取各种沟通行动来宣传这一研究项目。这些行动被认为对向不同受众广播项目成果非常重要，从而提高奖学金的影响力。

Efficient valorization of methane (CH4), the major component of natural gas, remains a significant challenge in catalysis. It is known that CH4 can be catalytically activated on two different active centers, through a radical pathway (dehydrogenation) or surfacestabilized M-CH3 pathway (deprotonation). This project aims to combine these two processes, through the design and synthesis of multifunctional catalysts, comprising of monovalent Zn+ sites and CuFe-oxo clusters, embedded within an omega zeolite. Through the application of such a strategy, it is thought that both methane deprotonation and dehydrogenation, could achievedsimultaneously. Previous literature has confirmed that omega zeolites can accommodate high concentrations of Cu or Fe active species, thus providing an abundance of active sites for converting CH4. A continuous-flow fixed-bed reaction setup is to be equipped for studying this reaction, to inhibit the overoxidation of CH3OH to less undesirable products. Ultimately, this project aims to (1) develop highly efficient and selective catalysts for CH4 conversion to CH3OH, and to (2) develop a better understanding on how different active sites promote methane activation and influence reaction selectivity in this process. Despite ongoing difficulties associated with the COVID-19 pandemic, various communicating actions will be employed to publicize this research project. Such actions are considered to be highly important for broadcasting the project outcomes to different audiences, thus elevating theimpact of the fellowship.