Automated Exploration\nof Heterogeneous Catalysis with\na Gas–Solid Nanoreactor

We present an automated method, gas–solid nanoreactor\nmolecular\ndynamics (GS-NMD), designed to explore reaction space and construct\nreaction networks for complex gas–solid heterogeneous catalysis\nsystems by integrating multiple acceleration techniques. Periodic\npulses were used to drive gas-phase molecules toward the catalyst\nsurface, accelerating adsorption and Eley–Rideal reactions.\nAdsorbed species were then subjected to metadynamics to overcome reaction\nbarriers associated with migration, Langmuir–Hinshelwood-type\nreactions, and desorption, using the root-mean-square deviations in\nCartesian space as collective variables. We demonstrate the efficiency\nof GS-NMD with the case of N<sub>2</sub> dissociation on Fe surfaces,\nshowing its ability to effectively screen for low-barrier reactions\nwithin a vast reaction space and distinct catalysts of different performances.\nAdditionally, we illustrate the method’s utility in constructing\neffective reaction networks for heterogeneous catalysis, exemplified\nby ammonia synthesis, which comprises only low-barrier elementary\nsteps. These results suggest that GS-NMD is a promising and efficient\ntool for the automated exploration of heterogeneous catalysis, enabling\nthe identification of the most favorable mechanisms and active sites\nfor gas–solid reactions.