N<sub>2</sub> cleavage by silylene and formation of H<sub>2</sub>Si(μ-N)<sub>2</sub>SiH<sub>2</sub>.
basic_science · Level V
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- Record sourced from PubMed, PMID 38719794.
- Also identified by DOI 10.1038/s41467-024-48064-z and PMC identifier 11078988.
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Abstract
Fixation and functionalisation of N<sub>2</sub> by main-group elements has remained scarce. Herein, we report a fixation and cleavage of the N ≡ N triple bond achieved in a dinitrogen (N<sub>2</sub>) matrix by the reaction of hydrogen and laser-ablated silicon atoms. The four-membered heterocycle H<sub>2</sub>Si(μ-N)<sub>2</sub>SiH<sub>2</sub>, the H<sub>2</sub>SiNN(H<sub>2</sub>) and HNSiNH complexes are characterized by infrared spectroscopy in conjunction with quantum-chemical calculations. The synergistic interaction of the two SiH<sub>2</sub> moieties with N<sub>2</sub> results in the formation of final product H<sub>2</sub>Si(μ-N)<sub>2</sub>SiH<sub>2</sub>, and theoretical calculations reveal the donation of electron density of Si to π* antibonding orbitals and the removal of electron density from the π bonding orbitals of N<sub>2</sub>, leading to cleave the non-polar and strong NN triple bond.