RuCatDAH: Rational design of Ruthenium Catalysts towards efficient Decomposition of Ammonia for Hydrogen production

高效分解氨（NH3）产生氢气（H2）是解决氢气储存和运输问题的理想途径。钌基催化剂是目前最先进的氨分解催化剂，但由于价格昂贵以及对催化剂结构与性能关系的认识不清，其催化性能难以满足大规模应用的要求，因此设计具有原子级活性中心的钌基催化剂是解决这一难题的有效途径。该项目将精确设计和合成负载型Ru催化剂，其尺寸范围从原子和亚纳米簇到纳米颗粒。多尺度Ru实体将改变催化剂表面上的NH3吸附、N-N形成和Ru-N解离，这可以通过一系列操作/原位X射线或红外光谱技术来探测。可能的中间体和反应机制（解离和缔合途径）将与这些操作方法结合密度泛函理论计算进行探索。在此基础上，同时高活性和最低限度的使用钌将实现进一步调制的最佳集成Ru网站与稀土氧化物（Zr掺杂CeO 2）表面。这些结果有望为欧盟委员会减少温室气体排放和促进氢经济的目标提供解决方案。尽管目前流行病的困难，各种沟通行动将被用来宣传这一研究项目，并提高奖学金的影响。

Efficient decomposition of ammonia (NH3) to generate hydrogen (H2) is an ideal approach to solving the H2 storage and transportation problem. Ru-based catalyst, the state-of-art catalyst toward NH3 decomposition, still fails to meet the requirements for large-scale applications due to the unaffordable cost and vague understanding of the catalyst structure-performance relationship.Designing catalysts with identical active centers on the atomic level is highly desired to mitigate this challenge. This project will precisely design and synthesize supported Ru catalysts with accurate sizes ranging from atomic and sub-nanometric clusters to nanoparticles. The multi-scale Ru entities will change the NH3 adsorption, N-N formation, and the Ru-N dissociation on the catalyst surface, which can be probed via a series of operando/in-situ X-ray or Infrared spectroscopic techniques. The possible intermediates and reaction mechanisms (Dissociative and Associative pathways) will be explored with those operando methods in combination with density-functional theory calculations. On this basis, the simultaneous high activity and minimum usage of Ru will be achieved by further modulating the optimal ensembled Ru sites with rare-earth oxide (Zr doped CeO2) surface. These results are expected to provide a solution toward the target of the European Commission in reducing greenhouse gas emissions and promoting the hydrogen economy. Despite ongoing pandemic difficulties, various communication actions will be employed to publicize this research project and elevate the fellowship's impact.