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The synthesis and characterisation of the S = 1/2 Fe(i) complex [Fe(depe) 2 ] + [BArF4] - ([ 1 ] + [BArF4] - ), and the facile reversible binding of N 2 and H 2 in both solution and the solid state to form the adducts [ 1 ·N 2 ] + and [ 1 ·H 2 ] + , are reported. Coordination of N 2 in THF is thermodynamically favourable under ambient conditions (1 atm; Δ G  298 = -4.9(1) kcal mol -1 ), while heterogenous binding is more favourable for H 2 than N 2 by a factor of ∼300. [ 1 ·H 2 ] + [BArF4] - represents a rare example of a well-defined, open-shell, non-classical dihydrogen complex, as corroborated by ESR spectroscopy. The rapid exchange between N 2 and H 2 coordination under ambient conditions is unique for a paramagnetic Fe complex.

chemical science

Reversible coordination of N2 and H2 to a homoleptic S = 1/2 Fe(<scp>i</scp>) diphosphine complex in solution and the solid state

Reversible coordination of N2 and H2 to a homoleptic S = 1/2 Fe(i) diphosphine complex in solution and the solid state

Reversible coordination of N₂ and H₂ to a homoleptic S = 1/2 Fe(i) diphosphine complex in solution and the solid state