针对直接氨燃料电池(DAFCs)阳极催化剂成本高、活性低、易中毒等缺点，围绕超临界CO2流体中单原子催化剂的形成机制及微观结构与催化性能间的关系等关键科学问题，本项目拟开展多孔碳负载单原子催化剂的可控合成及其氨气电氧化(AOR)性能研究。单原子催化剂拥有均一催化活性中心的同时具有最大化的金属原子的利用率，可以有效提高AOR催化活性和稳定性、降低成本。本项目将采用具有规整孔道结构的多孔碳为载体，通过配位点锚定和空间限域效应，采用超临界CO2方法结合热处理工艺，将金属原子负载在多孔碳表面获得目标产物。项目将探索此类材料形成过程中的表面结构、原子组成等信息，通过相关表征手段分析，推断催化材料形成机制，阐明催化剂微观结构对AOR性能的影响，研究催化反应过程中吸附中间产物的信息，结合理论计算，揭示其AOR催化机理。项目的实施不仅具有理论意义，而且在DAFCs领域具有潜在的应用前景。

Direct ammonia fuel cells (DAFCs) based on the ammonia electro-oxidation reaction (AOR) has attracted great attention recently and the electrocatalyst with low cost, high activity and stability is most improtant. Here, the supercritical CO2 method will be set up to design and fabricate the carbon supported single atom catalysts (SACs) and the AOR performance will also be investigated. The key scientific issues including the forming mechanism of the catalyst in supercritical CO2, the effect of microstructure on the AOR performance will be emphasized. By using spatial confinement strategy and coordination design strategy, the electrocatalysts will be obtained with porous carbon as supports via supercritical CO2 method followed by heat-treatment. SACs have attracted more and more attention as they have maximal atomic utilization as well as uniform coordination environments, thus providing a solution for the fabrication of AOR electrocatalysts with low cost and excellent performance. Advanced characterization techniques will be used to study the microstructure, morphology, atomic composition and the structure-function relationships between synergetic effects of heteroatoms doped supports and signle atoms versus catalytic properties will be demonstrated. The AOR mechanism of such catalysts will be investigated by the investigation of the intermediates obtained during the reaction combining with theoretical arithmetic. Studies here would be valuable not only in theory for SACs but also with potential value in engineering practice of DAFCs.