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Iridium (Ir) is an efficient catalyst for overall water splitting, yet its widespread utilization is hampered by the substantial cost and limited stability. Alloying Ir with heteroatoms can optimize the electronic structure of the catalyst and reduce the required amount of Ir. Compared to solid solution alloys, Ir‐based intermetallic compounds (IMCs) with ordered and stronger Ir‐heteroatom bonds exhibit...