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

CuFe 簇上的单点 Zn 用于甲烷选择性氧化为甲醇

• 批准号: EP/X021734/1
• 负责人: Bin Zhang
• 金额: $ 14.15万
• 依托单位: CARDIFF UNIVERSITY
• 依托单位国家: 英国
• 项目类别: Fellowship
• 财政年份: 2023
• 资助国家: 英国
• 起止时间: 2023 至 无数据
• 项目状态: 未结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FX021734%2F1
• 关键词: Single; site; Zn+; CuFe; clusters

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.

天然气的主要成分甲烷（CH4）的有效增值仍然是催化领域的重大挑战。众所周知，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激活。该项目旨在通过设计和合成多功能催化剂将这两个过程结合起来，该催化剂由单价 Zn+ 位点和嵌入 omega 沸石内的 CuFe-oxo 簇组成。通过应用这种策略，甲烷去质子化和脱氢可以同时实现。先前的文献已证实omega沸石可以容纳高浓度的Cu或Fe活性物质，从而为转化CH4提供丰富的活性位点。将配备连续流固定床反应装置来研究该反应，以抑制 CH3OH 过度氧化成较少的不需要的产物。最终，该项目的目标是 (1) 开发用于将 CH4 转化为 CH3OH 的高效和选择性催化剂，以及 (2) 更好地了解不同活性位点如何促进甲烷活化并影响该过程中的反应选择性。尽管与 COVID-19 大流行相关的困难持续存在，但仍将采取各种沟通行动来宣传该研究项目。这些行动被认为对于向不同受众传播项目成果非常重要，从而提高了奖学金的影响力。