Well-defined model systems are needed for better understanding of the relationship between optical, electronic, magnetic, and catalytic properties of nanoparticles and their structure. Chemical synthesis of metal nanoparticles results in large size and shape dispersion and lack of lateral order. In contrast, conventional top-down lithography techniques provide control over the lateral order and dimensions. However, they are either limited in resolution or have low throughput and therefore do not enable the large patterning area needed to obtain good signal-to-noise ratio in common analytical and characterization techniques. Extreme ultraviolet (EUV) lithography has the throughput and simplicity advantages of photolithography as well as high resolution due to its wavelength. Using EUV achromatic Talbot lithography, we have obtained 15 nm particle arrays with a periodicity of about 100 nm over an area of several square centimeters with high-throughput enabling the use of nanotechnology for fabrication of model systems to study large ensembles of well-defined identical nanoparticles with a density of 10(10) particles cm(-2).

We present a novel electrochemical flow cell based on a wall-jet configuration to carry out electrochemical investigations under controlled mass transport conditions. The described setup can be applied for investigations similar to those performed with a common rotating disc electrode setup but allows the use of non-conductive and square substrates. This setup thus opens the possibility for the characterization of a new range of materials on a broad range of substrates. Cyclic voltammograms were recorded to assess the cleanliness and good saturation of the cell with inert gas. The performance of the flow cell regarding hydrodynamic experiments was evaluated by probing the oxygen reduction reaction on differently prepared platinum catalysts, including Pt on non-conductive substrates. The high reproducibility of the limiting currents for these samples demonstrates the good functionality, adaptability, and flexibility of the cell.

We present numerical studies of the flow profile and electrode currents for the hydrogen oxidation and oxygen reduction reactions in an electrochemical flow cell. Koutecký-Levich type equations are obtained by partitioning the electrode surface into flow profile regimes and their correlation to idealized wall-jet and channel electrode geometries. The precision of several Koutecký-Levich type equations is evaluated and it is shown that differences between the most commonly applied equations are negligible within the range of flow rates studied and are surpassed by experimental errors.

We present recent developments in top-down nanofabrication that have found application in catalysis research. To unravel the complexity of catalytic systems, the design and use of models with control of size, morphology, shape and inter-particle distances is a necessity. The study of well-defined and ordered nanoparticles on a support contributes to the understanding of complex phenomena that govern reactions in heterogeneous and electro-catalysis. We review the strengths and limitations of different nanolithography methods such as electron beam lithography (EBL), photolithography, extreme ultraviolet (EUV) lithography and colloidal lithography for the creation of such highly tunable catalytic model systems and their applications in catalysis. Innovative strategies have enabled particle sizes reaching dimensions below 10 nm. It is now possible to create pairs of particles with distance controlled with an extremely high precision in the order of one nanometer. We discuss our approach to study these model systems at the single-particle level using X-ray absorption spectroscopy and show new ways to fabricate arrays of single nanoparticles or nanoparticles in pairs over a large area using EBL and EUV-achromatic Talbot lithography. These advancements have provided new insights into the active sites in metal catalysts and enhanced the understanding of the role of inter-particle interactions and catalyst supports, such as in the phenomenon of hydrogen spillover. We present a perspective on future directions for employing top-down nanofabrication in heterogeneous and electrocatalysis. The rapid development in nanofabrication and characterization methods will continue to have an impact on understanding of complex catalytic processes.

No abstract