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Addressing the implications of intermittent operation on process and plant operation This first requires investigations into the effect of variable operating conditions (particularly tem- perature, pressure, and gas composition) on catalyst activity, lifetime, surface morphology, and sensitivity to impurities. As the process is scaled up, plant-level optimization will also be required based on the dynamics of the specific source of renewable electricity as discussed in Section 9. Associated research needs include • Developing technology to make highly purified, pressurized N2 (5 year goal) • Developing technology to store/buffer H2 or H2/N2 mixtures at high pressure (5 year goal) • Handling of prolonged no-feed situations where e.g. week-long periods of no wind/sun require shutdown or throttle-down of the Haber-Bosch reactor (5 year goal) Discovering catalysts for ammonia synthesis at lower temperatures Theoretical studies have demonstrated that catalyst activity is limited by a balance between N2 dissociation and further hydrogenation of the atomic nitrogen adsorbed on the surface [5]. The N2 dissociation barrier (EN−N) can be directly linked to the energy of the final state of the elementary step in terms of atomic N binding energy (EN ). A strong binding surface will have a low barrier for N2 dissociation but will bind the N too strongly such that it will be poisoned by nitrogen species. A weak binding surface will be unable to activate N2 at a sufficient rate. This is illustrated in Figure 5.2, which shows the rate calculated with this mechanism and a mean-field kinetic model as a function of EN–N and EN. As shown, there exists a clear linear scaling relation between EN−N and EN for various transition metals. This means that a single variable is enough to define the catalyst activity, as shown in Figure 5.2b. Note that these results are consistent with the experimental observation that iron and ruthenium are the best ammonia synthesis catalysts [6]. Figure 5.2a indicates that the optimum for catalyst activity (shown in red) is far from the scaling line formed by the transition metal surfaces. It is therefore necessary to find means to break the scaling relation in order to discover significantly more active catalysts that can operate at lower temperatures. Below are two possible research directions that may lead to the discovery of active sites that do not obey this scaling relationship: • Synthesis of unique active sites where the relationship between transition state and final, dissociated state is different than on transition metals. • Design of a dynamically generated active site involving the reversible adsorption of co- adsorbed species, such as sulfur, fluorine, or oxygen that breaks the scaling relations between reaction intermediates. This idea is inspired by the nitrogenase enzyme [7]. 52PDF Image | sustainable production of fuels and chemicals
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