An iron diphosphineborane platform that was previously reported to facilitate a high degree of N-2 functionalization is herein shown to effect reductive CO coupling. Disilylation of an iron dicarbonyl precursor furnishes a structurally unprecedented iron dicarbyne complex. Several complexes related to this process are also characterized which allows for a comparative analysis of their respective Fe-B and Fe-C bonding. Facile hydrogenation of the iron dicarbyne at ambient temperature and 1 atm H-2 results in release of a CO-derived olefin.