Insights into CO2 Hydrogenation: Tuning the Selectivity towards Alcohols by Investigating Ni-Fe Bimetallic Catalysts

深入了解 CO2 加氢：通过研究 Ni-Fe 双金属催化剂调整醇的选择性

• 批准号: 452243354
• 负责人: Dr. Nina Sharmen Genz
• 金额: --
• 依托单位: Inorganic Chemistry and Catalysis
• 依托单位国家: 德国
• 项目类别: WBP Fellowship
• 财政年份: 2020
• 资助国家: 德国
• 起止时间: 2019-12-31 至 2022-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/452243354?language=en
• 关键词: Insights; into; CO2; Hydrogenation; Tuning

Rising atmospheric CO2 concentration constitutes one of the most challenging problems of today’s society. In view of the proceeding climate change and increasing awareness of its associated consequences, CO2 conversion into fuels and chemicals became a highly relevant topic. Here, hydrogenation of CO2 over non-noble, abundant, and relatively inexpensive metal catalysts constitutes a major advance. One key to conversion of the greenhouse gas CO2 into value-added products is the design of efficient and selective catalysts.Yet, in catalysis research, seeking more efficient and selective catalysts is an ongoing challenge. Rational catalyst design requires a fundamental understanding of the currently applied catalysts and of the reaction mechanism. Such a fundamental understanding can only be deduced by combining various analysis methods, as each method only provides particular information. Additionally, the analysis methods should be applied in situ, under reaction conditions, and operando, by combining several in situ methods, to understand the catalysts under realistic working conditions.For CO2 conversion to methane, Ni-based catalysts are commonly desired due to their high activity and selectivity. However, for CO2 hydrogenation towards alcohols, including long-chain alcohols, the optimal catalyst material is not yet found. Long-chain alcohols are required for various applications in industry and daily life, like as fuels. One possibility to redirect the selectivity in CO2 hydrogenation towards long-chain alcohols over Ni-based catalysts is to combine Ni with another metal, e.g. Fe, by taking advantage of the activity of Ni and the selectivity of Fe in a combined fashion.The main objective of this project is to tune the selectivity in CO2 hydrogenation towards alcohols by applying Ni-Fe/SiO2 catalysts and to gain a fundamental understanding of structure-function correlations of these catalysts. A multifaceted approach will be applied for gaining insights into these bimetallic catalysts at different levels. By doing so, various analysis methods will synergistically corroborate each other. For achieving this, the project will be built up on four pillars: catalysts synthesis and evaluation, detailed structural characterization, light spectroscopy, and X-ray based spectroscopy. Only the combination of the expected results of all four pillars will allow to elucidate the whole picture of the complex Ni-Fe/SiO2 catalysts. This will comprise the successful catalysts synthesis and the understanding of resulted structures and their evolutions, the reaction mechanism, structure sensitive effects, and finally the parameters for tuning the selectivity towards alcohols. Eventually, this multifaceted approach will enable to deduce a general guideline to design next generation bimetallic catalysts for going one step forward in CO2 hydrogenation towards long-chain alcohols.

大气中二氧化碳浓度的上升是当今社会最具挑战性的问题之一。鉴于正在发生的气候变化以及人们对其相关后果的认识不断提高，将二氧化碳转化为燃料和化学品已成为一个高度相关的议题。在这里，在非贵金属、丰富且相对便宜的金属催化剂上的CO2加氢构成了一个主要的进步。将温室气体CO2转化为高附加值产品的关键之一是设计高效、高选择性的催化剂，然而，在催化研究中，寻求更高效、更高选择性的催化剂是一个持续的挑战。合理的催化剂设计需要对目前应用的催化剂和反应机理有基本的了解。这种基本的理解只能通过结合各种分析方法来推导，因为每种方法只提供特定的信息。镍基催化剂因其高活性和高选择性而被广泛应用于CO2转化制甲烷反应中。然而，对于CO2加氢生成醇类（包括长链醇），尚未找到最佳催化剂材料，工业和日常生活中的各种应用都需要长链醇，例如作为燃料。在基于Ni的催化剂上将CO2氢化中的选择性重新导向长链醇的一种可能性是将Ni与另一种金属例如Fe组合，本课题的主要目的是利用Ni的活性和Fe的选择性来调节CO2加氢制醇的选择性，SiO2催化剂，并获得这些催化剂的结构-功能相关性的基本理解。将采用多方面的方法，在不同层面深入了解这些可持续发展的催化剂。通过这样做，各种分析方法将相互协同证实。为了实现这一目标，该项目将建立在四个支柱上：催化剂合成和评估，详细的结构表征，光谱学和X射线光谱学。只有所有四个支柱的预期结果的组合才能阐明复合Ni-Fe/SiO2催化剂的全貌。这将包括成功的催化剂合成和理解所产生的结构和它们的演变，反应机理，结构敏感性的影响，最后调整对醇的选择性的参数。最终，这种多方面的方法将能够推导出一个通用的指导方针，以设计下一代加氢催化剂，使二氧化碳加氢向长链醇迈进一步。