Altering the rate-determining step over cobalt single clusters leading to highly efficient ammonia synthesis.

ABSTRACT: Activation of high-energy triple-bonds of N₂ is the most significant bottleneck of ammonia synthesis under ambient conditions. Here, by importing cobalt single clusters as strong electron-donating promoter into the catalyst, the rate-determining step of ammonia synthesis is altered to the subsequent proton addition so that the barrier of N₂ dissociation can be successfully overcome. As revealed by density functional theory calculations, the N₂ dissociation becomes exothermic over the cobalt single cluster upon the strong electron backdonation from metal to the N₂ antibonding orbitals. The energy barrier of the positively shifted rate-determining step is also greatly reduced. At the same time, advanced sampling molecular dynamics simulations indic

SUBMITTER: Liu S 

PROVIDER: S-EPMC8288418 | biostudies-literature | 2021 May

REPOSITORIES: biostudies-literature