By combining experimental measurements with ab initio molecular dynamics simulations, we provide the first microscopic description of the interaction between metal surfaces and a low-temperature nitrogen-hydrogen plasma. Our study focuses on the dissociation of hydrogen and nitrogen as the main activation route. We find that ammonia forms via an Eley-Rideal mechanism where atomic nitrogen abstracts hydrogen from the catalyst surface to form ammonia on an extremely short time scale (a few picoseconds). On copper, ammonia formation occurs via the interaction between plasma-produced atomic nitrogen and the H-terminated surface. On platinum, however, we find that surface saturation with NH groups is necessary for ammonia production to occur. Regardless of the metal surface, the reaction is limited by the mass transport of atomic nitrogen, consistent with the weak dependence on catalyst material that we observe and has been reported by several other groups. This study represents a significant step toward achieving a mechanistic, microscopic-scale understanding of catalytic processes activated in low-temperature plasma environments.