The active site of the all-iron hydrogenase which catalyses hydrogen evolution / uptake is comprised of a di-iron sub-site linked to an {4Fe4S} – cubane cluster. The synthesis of sub-site analogues and thence a free-standing sub-site/cluster assembly possessing key structural elements of the catalytic H-centre machinery will be described. How such iron sulfur materials might offer the prospect of developing new electrocatalysts to replace platinum group metals in fuel cell applications will be discussed.