Surface\nSingle-Cluster Catalyst for N₂‑to-NH₃ Thermal Conversion

Abstract

The\nammonia synthesis from N₂ is of vital importance,\nwith imitating biological nitrogen fixation attracted much interest.\nHerein, we investigate the catalytic mechanisms of N₂-to-NH₃ thermal conversion on the singly dispersed bimetallic catalyst\nRh₁Co₃/CoO­(011), and find that the preferred\npathway is an associative mechanism analogous to the biological process,\nin which alternating hydrogenations of the N₂ occur, with\nH₂ activation on both metal sites. We propose that the\nsingly dispersed bimetallic M₁A_<i>n</i> catalyst, in which the doped metal atom M substitutes an oxygen\natom on the oxide surface of metal A, serves as a new surface single-cluster\ncatalyst (SCC) design platform for the biomimetic N₂-to-NH₃ thermal conversion. The catalytic ability of M₁A_<i>n</i> catalyst is attributed to both the\ncharge buffer capacity of doped metal M and the complementary role\nof synergic metal A in catalysis. Our work provides insights and guidelines\nfor further optimizing the M₁A_<i>n</i> catalyst.