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From the discovery of Fe2(CO)9 in 1905 to the intensive post-millennium study of dithiolate-bridged diiron complexes as biomimics of the active site of [FeFe]-hydrogenases, over the past century the diiron centre has been the most studied of binuclear systems. In this chapter we will focus on the synthesis, structure, bonding and reactivity of Fe2(CO)9, and derivatives based on the replacement or removal of one or more of the bridging carbonyl ligands.

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