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

高效分解氨(NH3)生成氢气(H2)是解决H2储存和运输问题的理想途径。铀基催化剂是目前最先进的NH3分解催化剂，但由于成本过高以及对催化剂结构与性能关系的认识不清，目前仍不能满足大规模应用的要求，因此迫切需要在原子水平上设计出具有相同活性中心的催化剂来缓解这一挑战。该项目将精确地设计和合成具有准确尺寸的负载型Ru催化剂，范围从原子和亚纳米团簇到纳米颗粒。多尺度Ru实体将改变催化剂表面NH3的吸附、N-N的生成和Ru-N的解离，这可以通过一系列的操纵面/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理(解离和缔合途径)将结合密度泛函理论计算用这些操作数方法来探索。在此基础上，进一步用稀土氧化物(Zr掺杂CeO2)对优化的Ru位进行调控，可以实现Ru的高活性和最低用量的同时。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。尽管疫情仍在继续，但仍将采取各种沟通行动来宣传这一研究项目，并提高研究基金的影响力。

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.