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.

甲烷（CH4）是天然气的主要组成部分，其高效增值仍然是催化领域的一个重大挑战。众所周知，CH4可以通过自由基途径（脱氢）或表面建立的M-CH3途径（去质子化）在两个不同的活性中心上被催化活化。该项目旨在结合这两个过程，通过设计和合成多功能催化剂，包括单价Zn+位点和CuFe-oxo簇，嵌入欧米茄沸石中。通过该策略的应用，可以同时实现甲烷的去质子化和脱氢。先前的文献已经证实，omega沸石可以容纳高浓度的Cu或Fe活性物质，从而为转化CH4提供了丰富的活性位点。研究该反应需配备连续流动固定床反应装置，以抑制CH3OH过度氧化生成较少的不良产物。本项目的最终目标是：(1)开发高效、选择性的CH4转化为CH3OH催化剂；(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大流行相关的困难仍然存在，但将采用各种沟通行动来宣传该研究项目。这些行动被认为对向不同的受众传播项目成果非常重要，从而提高奖学金的影响。