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

RuCatDAH：合理设计钌催化剂，实现氨高效分解制氢

• 批准号: EP/Y024931/1
• 负责人: Feng Ryan Wang
• 金额: $ 23.84万
• 依托单位: University College London
• 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%2FY024931%2F1
• 关键词: RuCatDAH; Rational; design; Ruthenium; Catalysts

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.

氨（NH3）高效分解生成氢气（H2）是解决氢气储运问题的理想途径。钌基催化剂是目前最先进的NH3分解催化剂，但由于成本过高和对催化剂结构-性能关系的认识不明确，仍不能满足大规模应用的要求。在原子水平上设计具有相同活性中心的催化剂是缓解这一挑战的迫切需要。该项目将精确地设计和合成负载钌催化剂，具有精确的大小，从原子和亚纳米簇到纳米颗粒。多尺度Ru实体会改变NH3在催化剂表面的吸附、N-N的形成和Ru- n的解离，这可以通过一系列的operando/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（解离和联想途径）将与这些operando方法结合密度泛函理论计算进行探讨。在此基础上，通过进一步用稀土氧化物（Zr掺杂CeO2）表面调制最佳包合Ru位点，可以同时实现Ru的高活性和最小使用量。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。尽管目前面临流行病方面的困难，但将采取各种传播行动来宣传这一研究项目并提高研究金的影响。