Prototyping of catalyst pore-systems by a combined synthetic, analytical and computational approach: Application to mesoporous TiO2

• Mesoporous TiO2 layer synthesized using nanocasting techniques.
• 3D morphology of pore-space analyzed by electron tomography.
• Pore size distribution observed in reconstructed tomograms matches experimental sorption data.
• Anisotropic diffusion coefficients evaluated by diffusion flux simulation in 3D medium.
• Parametric study revealed effects of templated pore size on model reactor performance.

During the last decade, quantum-chemical calculations of surface reactions have become well established for the design of catalytic sites. However, the corresponding methods allowing optimization of adequate pore structures for catalyst supports have so far not reached the same level of sophistication. This holds in particular for realistic pore systems that can be practically synthesized with a reasonable effort.We propose a strategy that enables virtual prototyping and computational optimization of the pore system of a solid catalyst. The method combines template-assisted synthesis of porous metal oxides with tunable pore-space morphology, 3D imaging of the catalysts nanostructure by the state-of-the-art electron tomography in HAADF STEM mode, and multi-scale mathematical modeling that provides computational evaluation of the pore size distribution, effective diffusivity and tortuosity in the reconstructed system as well as macroscopic performance of the catalytic layer in terms of reactant conversion. This general approach is demonstrated on mesoporous TiO2 layers.