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NANOPARTCAT Report Summary

Project ID: 338846
Funded under: FP7-IDEAS-ERC
Country: Netherlands

Mid-Term Report Summary - NANOPARTCAT (Supported Nanoparticles for Catalysis: Genesis and Dynamics in the Liquid Phase)

Supported metal nanoparticles, typically 1-10 nm in size, are used as catalysts to accelerate and steer chemical conversions to produce, e.g., transportation fuels, chemicals and medicines. This class of catalysts is also essential to shift from fossil fuels to a society based on renewable energy (biomass, sunlight). Albeit of eminent importance, supported metal catalysts are almost exclusively synthesized in liquid-phase processes that have been often considered ‘an art rather than a science’. Although recent insights from our laboratory and others on the fundamentals of catalysts synthesis are impressive, the lack of methodology to investigate directly the formation of supported nanoparticles in the liquid phase hampers progress.

The key objective of this proposal is to image and thereby obtain a detailed understanding of both the genesis (synthesis) and the dynamics (catalysis) of supported metal nanoparticles in the liquid phase with nanometer resolution and in real time. To this end we have combined two developments that are (1) a liquid-phase in situ cell for use in a transmission electron microscope (TEM) with (2) the element specificity of a so-called Super-EDX that provides element specific images with nanometer resolution using a unique detector system for X-rays. In this way we want to image in the liquid phase the nucleation and growth of nanoparticles on a support.

In project 1 we have focused on acquiring the equipment and developing expertise of TEM in liquid phase. First experiments have focused on one of the most important support materials in catalysis, i.e. silica, dispersed in water. Effects of the electron beam showed possibilities to affect the shape and the size of silica particles which has led to a first publication.

In projects 2 we have studied the synthesis of so-called bifunctional catalyst that contain both metal (Pt) and acid (zeolite) sites. By careful control for the first time we have been able to locate Pt either on the alumina or in the zeolite in composite support materials that contain alumina and zeolite. For the former system we have realized so-called ‘nanoscale intimacy’ of Pt and acid sites and in the latter ‘closest intimacy’. For 50 years in catalysis closest intimacy was thought to be most beneficial for activity and selectivity for hydrocarbon conversion catalysts. On the contrary, we have shown that for n-nonadecane cracking nanoscale intimacy led to lower undesired gas formation. This major breakthrough in catalysis has been published in Nature in December 2015. The newly acquired Super-EDX obtained with ERC support has been essential to achieve these groundbreaking results.

In project 3 we study iron nanocrystals on carbon nanotube support materials. These nanocrystals have been previously synthesized and their attachment to the support is studied in real time. It has been found that there are great effects of the functionalization of the carbon nanotubes on the extent to which the iron nanocrystal attach. Furthermore, their activity in synthesis gas conversion to lower olefins is very different upon support functionalization.

In project 4 we are in the process of moderating beam effects by changing solvent, beam intensity and support material. First results show beneficial effects of solvents other than water and oxides other than silica. For example titania is very stable in water and gold supported on titania has been studied showing dynamics of gold migration and nanoparticle growth to be absent in water and present in water with diethylenediamine dissolved. This provides a great basis for further studies in liquid-phase TEM.

In summary, we have made great strides in rational design, synthesis, characterization and functionality of advanced catalysts based on supported nanoparticles. The ERC-funded team of PhD students is now in full swing and we look forward to more exciting results.

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