Molecular design and X-ray spectroscopy of & on iron nanocluster catalysts

我们星球上的有氧条件使氧化物质的积累成为可能，而还原的化学物质构成了最有价值的能量载体。未来能源丰富的资源短缺使有效的减量化转变成为最大的科学挑战之一。该项目结合了最丰富的过渡金属铁在具有挑战性的还原转化中的作用和先进的基于同步加速器的表征技术。这项合作努力的成果将对现代化学合成/催化、材料和能源研究以及硬x射线的应用产生重大影响，以了解和改进这些系统。与贵金属技术相比，我们的努力利用了铁催化剂更高的还原能力和更强的可持续性。然而，设计活性的低价铁催化剂，实现新的催化反应，及其机理的理解将只有通过控制生成和有效稳定的还原铁种才有可能。重点将放在铁(0)纳米粒子与表面活性配体和溶剂系统之间相互作用的性质上，这些系统调节催化剂的立体电子性能。我们讨论了在溶液中自下而上合成铁(0)纳米粒子的各种方法，包括。将研究与制造有价值的化学品和材料最相关的催化反应（还原，氢化，去功能化等）。利用硬x射线进行详细的光谱研究，旨在了解合成参数与铁纳米颗粒的尺寸、表面性质和氧化态之间的相互作用，以及它们在纳米颗粒合成和催化反应过程中的动态变化。这个合作项目远远超出了化学合成领域，进入了与可持续生产和能源技术直接相关的材料研究、光谱和溶剂技术。我们的跨学科项目提供了新的还原铁催化剂，新的还原协议和新的光谱方法。

The aerobic conditions on our planet have enabled the accumulation of oxidized matter whereas reduced chemicals constitute the most valuable energy carriers. Future shortages of energy-rich resources make efficient reductive transformations one of the greatest scientific challenges. This project combines the action of the most abundant transition metal iron in challenging reductive transformations and advanced synchrotron-based characterization techniques. The outcomes of this collaborative effort will have major implications for modern chemical synthesis/catalysis and materials and energy research as well as the application of hard X-ray to understand and improve such systems. Our endeavour capitalizes on the higher reducing power and enhanced sustainability of iron catalysts over noble metal technologies. However, the design of active low-valent Fe catalysts, the realization of new catalytic reactions, and their mechanistic understanding will only be possible through the controlled generation and effective stabilization of reduced Fe species. Major emphasis will be placed on the nature of the interaction between iron(0) nano-particles and surface-active ligand and solvent systems that modulate the stereo-electronic properties of the catalyst. We address various approaches to the bottom-up synthesis of Fe(0) nanoparticles in solution, including. Catalytic reactions of utmost relevance to the manufacture of valuable chemicals and materials will be studied (reductions, hydrogenations, defunctionalizations etc.). Detailed spectroscopic investigations with hard X-rays aim at understanding the interplay between synthesis parameters and the size, surface properties and oxidation state of the iron nanoparticles and their dynamic changes during the nanoparticle synthesis and catalytic reactions. This collaborative project extends well beyond the realm of chemical synthesis into materials research, spectroscopy and solvent technologies with direct relevance to sustainable production and energy technologies. Our interdisciplinary program provides new sets of reducing iron catalysts, new reduction protocols, and new spectroscopic methods.