In the future, (electro‐)chemical catalysts will have to be more tolerant towards a varying supply of energy and raw materials. This is mainly due to the fluctuating nature of renewable energies. For example, power‐to‐chemical processes require a shift from steady‐state operation towards operation under dynamic reaction conditions. This brings along a number of demands for the design of both catalysts and reactors, because it is well‐known that the structure of catalysts is very dynamic. However, in‐depth studies of catalysts and catalytic reactors under such transient conditions have only started recently. This requires studies and advances in the fields of 1) operando spectroscopy including time‐resolved methods, 2) theory with predictive quality, 3) kinetic modelling, 4) design of catalysts by appropriate preparation concepts, and 5) novel/modular reactor designs. An intensive exchange between these scientific disciplines will enable a substantial gain of fundamental knowledge which is urgently required. This concept article highlights recent developments, challenges, and future directions for understanding catalysts under dynamic reaction conditions.
PFG NMR has been applied to study intracrystalline diffusion in USY zeolite as well as in the parent ammonium-ion exchanged zeolite Y used to produce the USY by zeolite steaming. The diffusion studies have been performed for a broad range of molecular displacements and with two different types of probe molecules (n-octane and 1,3,5-triisopropylbenzene) having critical molecular diameters smaller and larger than the openings of the zeolite micropores. Our experimental data unambiguously show that, in contrast to what is usually assumed in the literature, the intracrystalline mesopores do not significantly affect intracrystalline diffusion in USY. This result indicates that the intracrystalline mesopores of USY zeolite do not form a connected network, which would allow diffusion through crystals only via mesopores.
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