Formation and structures of unsaturated cobalt hydride complexes, using 50% thermal ellipsoids. Carbon-bound hydrogen atoms are omitted for clarity. All cobalt-bound hydrogens were refined with isotropic thermal parameters. Selected bond lengths and bond angles follow; because compound 1 has three crystallographically independent dimers, ranges are listed here (details are in the Supporting Information). 1: Co-Co 2.472-2.481 Å, Co-N 1.962-1.993 Å, N-Co-N 95.4-96.5°. For 2: Co1-Co2 5.7386(7) Å, Co1-H1 1.84(2) Å, Co1-N11 1.9162(13) Å, Co1-N21 1.9164(12) Å, N11-Co1-N21 96.73(6)°, N11-Co1-H1 128.2(7)°, N21-Co1-H1 134.1(7)°, Co2-H2 1.78(2) Å, Co2-N14 1.9106(13) Å, Co2-N24 1.9121(13) Å, N14-Co2-N24 96.59(6)°, N14-Co2-H2 133.5(7)°, N24-Co2-H2 129.4(7)°.