AtomCat4Fuel: Atomically construction of AuPd catalyst for efficient CO2 hydrogenation to ethanol

AtomCat4Fuel：原子构建 AuPd 催化剂，用于高效 CO2 加氢生成乙醇

• 批准号: EP/Y029305/1
• 负责人: Graham Hutchings
• 金额: $ 23.84万
• 依托单位: CARDIFF UNIVERSITY
• 依托单位国家: 英国
• 项目类别: Fellowship
• 财政年份: 2024
• 资助国家: 英国
• 起止时间: 2024 至 无数据
• 项目状态: 未结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FY029305%2F1
• 关键词: AtomCat4Fuel; Atomically; construction; AuPd; catalyst

Climate change is arguably one of the most top challenges our planet facing during the 21st century, mainly due to huge amounts of greenhouse gas emissions in CO2 form to the atmosphere. In this regard, the catalytic upgradation of CO2 into fuels and high-value chemicals, e.g., ethanol, appears to be one of the most valuable solutions to address the overloaded CO2 in air. Catalytic CO2 hydrogenation to ethanol (CTE) not only contributes to slow down the global warming but also contributes to alleviate the global food shortage. Among various developed catalysts, Au- and Pd-based nano-materials emerge as one of the most effective catalysts for CO2 hydrogenation to ethanol, which deserves more research efforts. While the limited ethanol activity (TOF < 400 h-1) and relatively harsh reaction conditions (T greater than or equal to 200 oC, P > 3 MPa) preclude these works from industrialization. Herein, this proposal focuses on developing the strategies to maximize the atom utilization efficiency and the sites number of metal/adjacent oxygen vacancy, through atom-by-atom constructing atomically precise Au/Pd sites on oxygen-vacancy-rich My/TiO2-x (i.e., M=In3+, Fe3+), to further improve ethanol productivity under mild conditions. Furthermore, various operando spectroscopy techniques (e.g., operando X-ray absorption spectroscopy and steady-state isotopic transient kinetic analysis) will be integrated to identify the intermediates and mechanism of C-C coupling, thus establishing a clear structure-performance relationship and providing a rational guidance for the design of future CO2 catalysts, all of which will contribute to the ambitious goal of European Commission for reducing CO2 emissions from all sources by 80%-95% by 2050.

气候变化可以说是我们星球在 21 世纪面临的最严峻的挑战之一，这主要是由于大量以二氧化碳形式排放到大气中的温室气体造成的。在这方面，将二氧化碳催化升级为燃料和高价值化学品（例如乙醇）似乎是解决空气中二氧化碳超载的最有价值的解决方案之一。催化二氧化碳加氢制乙醇（CTE）不仅有助于减缓全球变暖，还有助于缓解全球粮食短缺。在各种已开发的催化剂中，金基和钯基纳米材料成为二氧化碳加氢制乙醇最有效的催化剂之一，值得更多的研究工作。然而有限的乙醇活性（TOF < 400 h-1）和相对苛刻的反应条件（T大于或等于200 oC，P > 3 MPa）阻碍了这些作品的工业化。在此，该提案的重点是通过在富含氧空位的 My/TiO2-x 上逐个原子构建原子精确的 Au/Pd 位点，开发最大化原子利用效率和金属/相邻氧空位位点数量的策略（即M=In3+、Fe3+），进一步提高温和条件下的乙醇生产率。此外，将整合各种原位光谱技术（例如原位X射线吸收光谱和稳态同位素瞬态动力学分析）来识别C-C偶联的中间体和机制，从而建立清晰的结构-性能关系，并提供合理的指导。未来二氧化碳催化剂的设计，所有这些都将有助于实现欧盟委员会的雄心勃勃的目标，即到 2050 年将所有来源的二氧化碳排放量减少 80%-95%。