FeH42(C3N4)6 crystallizes in the trigonal R3 space group. There are two inequivalent Fe sites. In the first Fe site, Fe(1) is bonded in an octahedral geometry to three equivalent N(16) and three equivalent N(8) atoms. All Fe(1)-N(16) bond lengths are 2.18 Å. All Fe(1)-N(8) bond lengths are 2.19 Å. In the second Fe site, Fe(2) is bonded in an octahedral geometry to three equivalent N(12) and three equivalent N(4) atoms. All Fe(2)-N(12) bond lengths are 2.18 Å. All Fe(2)-N(4) bond lengths are 2.19 Å. There are twelve inequivalent C sites. In the first C site, C(1) is bonded in a trigonal planar geometry to one N(1), one N(4), and one H(1) atom. The C(1)-N(1) bond length is 1.31 Å. The C(1)-N(4) bond length is 1.36 Å. The C(1)-H(1) bond length is 0.93 Å. In the second C site, C(2) is bonded in a trigonal planar geometry to one N(5), one N(8), and one H(2) atom. The C(2)-N(5) bond length is 1.30 Å. The C(2)-N(8) bond length is 1.34 Å. The C(2)-H(2) bond length is 0.93 Å. In the third C site, C(3) is bonded in a trigonal planar geometry to one N(12), one N(9), and one H(3) atom. The C(3)-N(12) bond length is 1.33 Å. The C(3)-N(9) bond length is 1.31 Å. The C(3)-H(3) bond length is 0.93 Å. In the fourth C site, C(4) is bonded in a trigonal planar geometry to one N(13), one N(16), and one H(4) atom. The C(4)-N(13) bond length is 1.32 Å. The C(4)-N(16) bond length is 1.35 Å. The C(4)-H(4) bond length is 0.93 Å. In the fifth C site, C(5) is bonded in a 5-coordinate geometry to one N(2), one H(11), one H(12), one H(5), and one H(6) atom. The C(5)-N(2) bond length is 1.46 Å. The C(5)-H(11) bond length is 0.97 Å. The C(5)-H(12) bond length is 0.97 Å. The C(5)-H(5) bond length is 0.97 Å. The C(5)-H(6) bond length is 0.97 Å. In the sixth C site, C(6) is bonded in a 3-coordinate geometry to one H(11), one H(7), and one H(8) atom. The C(6)-H(11) bond length is 1.24 Å. The C(6)-H(7) bond length is 0.97 Å. The C(6)-H(8) bond length is 0.97 Å. In the seventh C site, C(7) is bonded in a 5-coordinate geometry to one N(6), one H(10), one H(15), one H(16), and one H(9) atom. The C(7)-N(6) bond length is 1.46 Å. The C(7)-H(10) bond length is 0.97 Å. The C(7)-H(15) bond length is 0.97 Å. The C(7)-H(16) bond length is 0.97 Å. The C(7)-H(9) bond length is 0.97 Å. In the eighth C site, C(8) is bonded in a 4-coordinate geometry to one H(10), one H(13), one H(14), and one H(6) atom. The C(8)-H(10) bond length is 1.32 Å. The C(8)-H(13) bond length is 0.97 Å. The C(8)-H(14) bond length is 0.97 Å. The C(8)-H(6) bond length is 1.22 Å. In the ninth C site, C(9) is bonded in a 5-coordinate geometry to one N(10), one H(17), one H(18), one H(23), and one H(24) atom. The C(9)-N(10) bond length is 1.47 Å. The C(9)-H(17) bond length is 0.97 Å. The C(9)-H(18) bond length is 0.97 Å. The C(9)-H(23) bond length is 0.97 Å. The C(9)-H(24) bond length is 0.97 Å. In the tenth C site, C(10) is bonded in a 2-coordinate geometry to one H(19), one H(20), and one H(24) atom. The C(10)-H(19) bond length is 0.97 Å. The C(10)-H(20) bond length is 0.97 Å. The C(10)-H(24) bond length is 1.32 Å. In the eleventh C site, C(11) is bonded in a 5-coordinate geometry to one N(14), one H(21), one H(22), one H(27), and one H(28) atom. The C(11)-N(14) bond length is 1.44 Å. The C(11)-H(21) bond length is 0.97 Å. The C(11)-H(22) bond length is 0.97 Å. The C(11)-H(27) bond length is 0.97 Å. The C(11)-H(28) bond length is 0.97 Å. In the twelfth C site, C(12) is bonded in a 2-coordinate geometry to one H(17), one H(21), one H(25), and one H(26) atom. The C(12)-H(17) bond length is 1.31 Å. The C(12)-H(21) bond length is 1.27 Å. The C(12)-H(25) bond length is 0.97 Å. The C(12)-H(26) bond length is 0.97 Å. There are sixteen inequivalent N sites. In the first N site, N(1) is bonded in a distorted water-like geometry to one C(1) and one N(2) atom. The N(1)-N(2) bond length is 1.36 Å. In the second N site, N(2) is bonded in a distorted single-bond geometry to one C(5), one N(1), and one N(3) atom. The N(2)-N(3) bond length is 1.30 Å. In the third N site, N(3) is bonded in a water-like geometry to one N(2) and one N(4) atom. The N(3)-N(4) bond length is 1.32 Å. In the fourth N site, N(4) is bonded in a distorted trigonal planar geometry to one Fe(2), one C(1), and one N(3) atom. In the fifth N site, N(5) is bonded in a water-like geometry to one C(2) and one N(6) atom. The N(5)-N(6) bond length is 1.33 Å. In the sixth N site, N(6) is bonded in a distorted single-bond geometry to one C(7), one N(5), and one N(7) atom. The N(6)-N(7) bond length is 1.31 Å. In the seventh N site, N(7) is bonded in a water-like geometry to one N(6) and one N(8) atom. The N(7)-N(8) bond length is 1.31 Å. In the eighth N site, N(8) is bonded in a 3-coordinate geometry to one Fe(1), one C(2), and one N(7) atom. In the ninth N site, N(9) is bonded in a distorted water-like geometry to one C(3) and one N(10) atom. The N(9)-N(10) bond length is 1.33 Å. In the tenth N site, N(10) is bonded in a distorted single-bond geometry to one C(9), one N(11), and one N(9) atom. The N(10)-N(11) bond length is 1.29 Å. In the eleventh N site, N(11) is bonded in a water-like geometry to one N(10) and one N(12) atom. The N(11)-N(12) bond length is 1.32 Å. In the twelfth N site, N(12) is bonded in a distorted trigonal planar geometry to one Fe(2), one C(3), and one N(11) atom. In the thirteenth N site, N(13) is bonded in a water-like geometry to one C(4) and one N(14) atom. The N(13)-N(14) bond length is 1.29 Å. In the fourteenth N site, N(14) is bonded in a distorted single-bond geometry to one C(11), one N(13), and one N(15) atom. The N(14)-N(15) bond length is 1.32 Å. In the fifteenth N site, N(15) is bonded in a water-like geometry to one N(14) and one N(16) atom. The N(15)-N(16) bond length is 1.30 Å. In the sixteenth N site, N(16) is bonded in a distorted trigonal planar geometry to one Fe(1), one C(4), and one N(15) atom. There are twenty-eight inequivalent H sites. In the first H site, H(1) is bonded in a single-bond geometry to one C(1) atom. In the second H site, H(2) is bonded in a single-bond geometry to one C(2) atom. In the third H site, H(3) is bonded in a single-bond geometry to one C(3) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(4) atom. In the fifth H site, H(5) is bonded in a distorted single-bond geometry to one C(5) atom. In the sixth H site, H(6) is bonded in a distorted L-shaped geometry to one C(5) and one C(8) atom. In the seventh H site, H(7) is bonded in a single-bond geometry to one C(6) atom. In the eighth H site, H(8) is bonded in a single-bond geometry to one C(6) atom. In the ninth H site, H(9) is bonded in a distorted single-bond geometry to one C(7), one H(15), and one H(16) atom. The H(9)-H(15) bond length is 0.85 Å. The H(9)-H(16) bond length is 0.86 Å. In the tenth H site, H(10) is bonded in a 2-coordinate geometry to one C(7) and one C(8) atom. In the eleventh H site, H(11) is bonded in a 2-coordinate geometry to one C(5) and one C(6) atom. In the twelfth H site, H(12) is bonded in a distorted single-bond geometry to one C(5) atom. In the thirteenth H site, H(13) is bonded in a single-bond geometry to one C(8) atom. In the fourteenth H site, H(14) is bonded in a single-bond geometry to one C(8) atom. In the fifteenth H site, H(15) is bonded in a distorted single-bond geometry to one C(7) and one H(9) atom. In the sixteenth H site, H(16) is bonded in a distorted single-bond geometry to one C(7) and one H(9) atom. In the seventeenth H site, H(17) is bonded in a 3-coordinate geometry to one C(12), one C(9), and one H(23) atom. The H(17)-H(23) bond length is 0.88 Å. In the eighteenth H site, H(18) is bonded in a distorted single-bond geometry to one C(9) and one H(24) atom. The H(18)-H(24) bond length is 0.86 Å. In the nineteenth H site, H(19) is bonded in a single-bond geometry to one C(10) atom. In the twentieth H site, H(20) is bonded in a single-bond geometry to one C(10) atom. In the twenty-first H site, H(21) is bonded in a 2-coordinate geometry to one C(11) and one C(12) atom. In the twenty-second H site, H(22) is bonded in a distorted single-bond geometry to one C(11), one H(27), and one H(28) atom. The H(22)-H(27) bond length is 0.81 Å. The H(22)-H(28) bond length is 0.90 Å. In the twenty-third H site, H(23) is bonded in a distorted single-bond geometry to one C(9) and one H(17) atom. In the twenty-fourth H site, H(24) is bonded in a 3-coordinate geometry to one C(10), one C(9), and one H(18) atom. In the twenty-fifth H site, H(25) is bonded in a single-bond geometry to one C(12) atom. In the twenty-sixth H site, H(26) is bonded in a single-bond geometry to one C(12) atom. In the twenty-seventh H site, H(27) is bonded in a distorted single-bond geometry to one C(11) and one H(22) atom. In the twenty-eighth H site, H(28) is bonded in a distorted single-bond geometry to one C(11) and one H(22) atom. Linkers: 11 C.C.C1=NN=N[N]1.C1=NN=N[N]1.[CH2].[CH2] ,7 C.C.C1=NN=N[N]1.C1=NN=N[N]1.C=C. Metal clusters: 6 [Fe]. The MOF has largest included sphere 5.04 A, density 1.15 g/cm3, surface area 4559.62 m2/g, accessible volume 0.42 cm3/g