Mechanistic Inquisition on the Reduction of C₁₇Si(NH₂)₂ to NH₃: A DFT Study

Activation of molecular nitrogen by silicon-substituted cyclo[18]carbon and its ability to produce the C₁₇Si-(NH₂)₂ derivative, as the precursor of NH₃, has been recently reported. This specific acquisition has piqued an interest to investigate the possibility of NH₃ formation with further addition of H₂ molecules in the gaseous reaction media. The current investigations reported in this article show that two moles of molecular H₂ generate two molecules of NH₃ and a C₁₇Si-H₂ byproduct from its precursor. The catalyst gets restored by an in situ reaction between some unreacted C₁₇Si-N₂ and the byproduct in the media. This reaction also produces the next C₁₇Si-(NH)₂ adduct, which restarts the catalytic cycle for NH₃ production again.