Room-Temperature H₂ Splitting and N₂-Hydrogenation Induced by a Neutral Lu^II Complex.

Area of Science:

• Inorganic Chemistry
• Organometallic Chemistry
• Catalysis

Background:

• Direct splitting of H2 and N2 is crucial for ammonia synthesis but challenging.
• Lanthanide complexes have not previously shown this reactivity.

Purpose of the Study:

• To explore the reactivity of low-valent lanthanide species.
• To achieve direct H2 and N2 splitting using molecular lanthanide complexes.

Main Methods:

• Synthesis and characterization of a kinetically stable LuII complex.
• Experimental studies of H2 splitting and N2 binding.
• Density Functional Theory (DFT) calculations to corroborate findings.

Main Results:

• A novel divalent lutetium (LuII) complex was successfully isolated and characterized.
• The LuII complex demonstrated direct H2 splitting at room temperature.
• The complex also bound N2, forming a diazenido complex, which was subsequently hydrogenated to a LuIII-NH2 complex.

Conclusions:

• Low-valent molecular rare-earth metal complexes can achieve direct N2 hydrogenation and cleavage.
• This work introduces unprecedented reactivity for lanthanide chemistry.
• The findings open new avenues for catalytic ammonia synthesis and nitrogen fixation.