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[Ni(L(1))Fe((t)BuNC)4](PF6)2 is a robust Ni(II)Fe(II) complex that undergoes a reversible one-electron reduction. Spectroscopic and theoretical studies show that [Ni(L(1))Fe((t)BuNC)4](+) is an unprecedented Ni(I)Fe(II) species that reproduces the electronic configuration of the Ni-L state of the [NiFe] hydrogenases.

A Ni(i)Fe(ii) analogue of the Ni-L state of the active site of the [NiFe] hydrogenases