Fe(Co5N4)2 crystallizes in the monoclinic C2/m space group. Fe(1) is bonded in a square co-planar geometry to two equivalent N(3) and two equivalent N(4) atoms. There are five inequivalent Co sites. In the first Co site, Co(1) is bonded in a distorted T-shaped geometry to one N(1), one N(2), and one N(3) atom. In the second Co site, Co(2) is bonded to one N(2), two equivalent N(1), and two equivalent N(4) atoms to form a mixture of edge and corner-sharing CoN5 square pyramids. In the third Co site, Co(3) is bonded to one N(3), one N(4), and three equivalent N(2) atoms to form a mixture of edge and corner-sharing CoN5 square pyramids. In the fourth Co site, Co(4) is bonded to one N(3), two equivalent N(1), and two equivalent N(4) atoms to form a mixture of edge and corner-sharing CoN5 square pyramids. In the fifth Co site, Co(5) is bonded in a square co-planar geometry to one N(1), one N(2), and two equivalent N(3) atoms. There are four inequivalent N sites. In the first N site, N(1) is bonded to one Co(1), one Co(5), two equivalent Co(2), and two equivalent Co(4) atoms to form NCo6 octahedra that share  a cornercorner with one N(3)FeCo5 octahedra, corners with two equivalent N(1)Co6 octahedra, corners with two equivalent N(2)Co6 octahedra,  an edgeedge with one N(1)Co6 octahedra,  an edgeedge with one N(2)Co6 octahedra, edges with two equivalent N(3)FeCo5 octahedra, and edges with four equivalent N(4)FeCo5 octahedra. The corner-sharing octahedral tilt angles range from 5-24°. In the second N site, N(2) is bonded to one Co(1), one Co(2), one Co(5), and three equivalent Co(3) atoms to form NCo6 octahedra that share  a cornercorner with one N(4)FeCo5 octahedra, corners with two equivalent N(1)Co6 octahedra, corners with two equivalent N(2)Co6 octahedra,  an edgeedge with one N(1)Co6 octahedra, edges with two equivalent N(2)Co6 octahedra, edges with two equivalent N(4)FeCo5 octahedra, and edges with three equivalent N(3)FeCo5 octahedra. The corner-sharing octahedral tilt angles range from 5-14°. In the third N site, N(3) is bonded to one Fe(1), one Co(1), one Co(3), one Co(4), and two equivalent Co(5) atoms to form NFeCo5 octahedra that share  a cornercorner with one N(1)Co6 octahedra,  a cornercorner with one N(4)FeCo5 octahedra, corners with three equivalent N(3)FeCo5 octahedra, edges with two equivalent N(1)Co6 octahedra, edges with two equivalent N(4)FeCo5 octahedra, and edges with three equivalent N(2)Co6 octahedra. The corner-sharing octahedral tilt angles range from 0-24°. In the fourth N site, N(4) is bonded to one Fe(1), one Co(3), two equivalent Co(2), and two equivalent Co(4) atoms to form NFeCo5 octahedra that share  a cornercorner with one N(2)Co6 octahedra,  a cornercorner with one N(3)FeCo5 octahedra, corners with three equivalent N(4)FeCo5 octahedra,  an edgeedge with one N(4)FeCo5 octahedra, edges with two equivalent N(2)Co6 octahedra, edges with two equivalent N(3)FeCo5 octahedra, and edges with four equivalent N(1)Co6 octahedra. The corner-sharing octahedral tilt angles range from 0-14°.
Fe(Co5N4)2 crystallizes in the monoclinic C2/m space group. Fe(1) is bonded in a square co-planar geometry to two equivalent N(3) and two equivalent N(4) atoms. Both Fe(1)-N(3) bond lengths are 2.00 Å. Both Fe(1)-N(4) bond lengths are 1.92 Å. There are five inequivalent Co sites. In the first Co site, Co(1) is bonded in a distorted T-shaped geometry to one N(1), one N(2), and one N(3) atom. The Co(1)-N(1) bond length is 1.87 Å. The Co(1)-N(2) bond length is 1.87 Å. The Co(1)-N(3) bond length is 1.87 Å. In the second Co site, Co(2) is bonded to one N(2), two equivalent N(1), and two equivalent N(4) atoms to form a mixture of edge and corner-sharing CoN5 square pyramids. The Co(2)-N(2) bond length is 2.00 Å. Both Co(2)-N(1) bond lengths are 2.00 Å. Both Co(2)-N(4) bond lengths are 1.99 Å. In the third Co site, Co(3) is bonded to one N(3), one N(4), and three equivalent N(2) atoms to form a mixture of edge and corner-sharing CoN5 square pyramids. The Co(3)-N(3) bond length is 1.97 Å. The Co(3)-N(4) bond length is 1.95 Å. There is one shorter (1.96 Å) and two longer (1.98 Å) Co(3)-N(2) bond lengths. In the fourth Co site, Co(4) is bonded to one N(3), two equivalent N(1), and two equivalent N(4) atoms to form a mixture of edge and corner-sharing CoN5 square pyramids. The Co(4)-N(3) bond length is 2.02 Å. Both Co(4)-N(1) bond lengths are 2.00 Å. There is one shorter (1.93 Å) and one longer (2.09 Å) Co(4)-N(4) bond length. In the fifth Co site, Co(5) is bonded in a square co-planar geometry to one N(1), one N(2), and two equivalent N(3) atoms. The Co(5)-N(1) bond length is 1.91 Å. The Co(5)-N(2) bond length is 1.91 Å. Both Co(5)-N(3) bond lengths are 1.99 Å. There are four inequivalent N sites. In the first N site, N(1) is bonded to one Co(1), one Co(5), two equivalent Co(2), and two equivalent Co(4) atoms to form NCo6 octahedra that share  a cornercorner with one N(3)FeCo5 octahedra, corners with two equivalent N(1)Co6 octahedra, corners with two equivalent N(2)Co6 octahedra,  an edgeedge with one N(1)Co6 octahedra,  an edgeedge with one N(2)Co6 octahedra, edges with two equivalent N(3)FeCo5 octahedra, and edges with four equivalent N(4)FeCo5 octahedra. The corner-sharing octahedral tilt angles range from 5-24°. In the second N site, N(2) is bonded to one Co(1), one Co(2), one Co(5), and three equivalent Co(3) atoms to form NCo6 octahedra that share  a cornercorner with one N(4)FeCo5 octahedra, corners with two equivalent N(1)Co6 octahedra, corners with two equivalent N(2)Co6 octahedra,  an edgeedge with one N(1)Co6 octahedra, edges with two equivalent N(2)Co6 octahedra, edges with two equivalent N(4)FeCo5 octahedra, and edges with three equivalent N(3)FeCo5 octahedra. The corner-sharing octahedral tilt angles range from 5-14°. In the third N site, N(3) is bonded to one Fe(1), one Co(1), one Co(3), one Co(4), and two equivalent Co(5) atoms to form NFeCo5 octahedra that share  a cornercorner with one N(1)Co6 octahedra,  a cornercorner with one N(4)FeCo5 octahedra, corners with three equivalent N(3)FeCo5 octahedra, edges with two equivalent N(1)Co6 octahedra, edges with two equivalent N(4)FeCo5 octahedra, and edges with three equivalent N(2)Co6 octahedra. The corner-sharing octahedral tilt angles range from 0-24°. In the fourth N site, N(4) is bonded to one Fe(1), one Co(3), two equivalent Co(2), and two equivalent Co(4) atoms to form NFeCo5 octahedra that share  a cornercorner with one N(2)Co6 octahedra,  a cornercorner with one N(3)FeCo5 octahedra, corners with three equivalent N(4)FeCo5 octahedra,  an edgeedge with one N(4)FeCo5 octahedra, edges with two equivalent N(2)Co6 octahedra, edges with two equivalent N(3)FeCo5 octahedra, and edges with four equivalent N(1)Co6 octahedra. The corner-sharing octahedral tilt angles range from 0-14°.