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.

天然气的主要组成部分甲烷（CH4）的有效价值仍然是催化中的重大挑战。众所周知，CH4可以通过自由基途径（脱氢）或表面上的M-CH3途径（去质子化）在两个不同的活性中心上催化激活。该项目旨在通过设计和合成多功能催化剂，包括单价Zn+位点和Cufe-oxo簇，嵌入了欧米茄岩中。通过采用这种策略，人们认为甲烷去质子化和脱氢作用都可以相比实现。先前的文献已经证实，欧米茄沸石可以容纳高浓度的铜或fe活性物种，从而提供了大量的活性位点来转换CH4。连续流固定床反应的设置将配备用于研究该反应，以抑制CH3OH过度氧化对较低的不良产品的过度氧化。最终，该项目的目的是（1）为CH4转化为CH3OH的高效和选择性催化剂，并对（2）对不同的活性位点如何促进甲烷激活并影响此过程中的反应选择性有了更好的了解。尽管与19日大流行有关的困难持续存在，但仍将采取各种沟通行动来宣传该研究项目。这种行动被认为对于将项目成果广播给不同的受众非常重要，从而提高了研究金的影响。