The role of dynamics in heterogeneous catalysis: Surface diffusivity and N2 
decomposition on Fe(111)

Bonati , Luigi; Polino, Daniela; Pizzolitto, Cristina; Biasi, Pierdomenico; Eckert, Rene; Reitmeier, Stephan; Schlögl, Robert; Parrinello, Michele

doi:10.1073/pnas.2313023120

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The role of dynamics in heterogeneous catalysis: Surface diffusivity and N₂ decomposition on Fe(111)

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Schlögl, Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Citation

Bonati, L., Polino, D., Pizzolitto, C., Biasi, P., Eckert, R., Reitmeier, S., et al. (2023). The role of dynamics in heterogeneous catalysis: Surface diffusivity and N₂ decomposition on Fe(111). Proceedings of the National Academy of Sciences of the United States of America, 120(50): e231302312. doi:10.1073/pnas.2313023120.

Cite as: https://hdl.handle.net/21.11116/0000-000E-20C8-C

Abstract

Dynamics has long been recognized to play an important role in heterogeneous catalytic processes. However, until recently, it has been impossible to study their dynamical behavior at industry-relevant temperatures. Using a combination of machine learning potentials and advanced simulation techniques, we investigate the cleavage of the N₂ triple bond on the Fe(111) surface. We find that at low temperatures our results agree with the well-established picture. However, if we increase the temperature to reach operando conditions, the surface undergoes a global dynamical change and the step structure of the Fe(111) surface is destabilized. The catalytic sites, traditionally associated with this surface, appear and disappear continuously. Our simulations illuminate the danger of extrapolating low-temperature results to operando conditions and indicate that the catalytic activity can only be inferred from calculations that take dynamics fully into account. More than that, they show that it is the transition to this highly fluctuating interfacial environment that drives the catalytic process.