Ni3C14P4H24(NO9)2 crystallizes in the triclinic P1 space group. There are three inequivalent Ni sites. In the first Ni site, Ni(1) is bonded to one O(1), one O(15), one O(16), one O(2), one O(7), and one O(8) atom to form NiO6 octahedra that share  a cornercorner with one P(1)CO3 tetrahedra,  a cornercorner with one P(2)CO3 tetrahedra,  a cornercorner with one P(3)CO3 tetrahedra, and  a cornercorner with one P(4)CO3 tetrahedra. The Ni(1)-O(1) bond length is 2.01 Å. The Ni(1)-O(15) bond length is 2.14 Å. The Ni(1)-O(16) bond length is 2.13 Å. The Ni(1)-O(2) bond length is 2.01 Å. The Ni(1)-O(7) bond length is 2.06 Å. The Ni(1)-O(8) bond length is 2.06 Å. In the second Ni site, Ni(2) is bonded to one O(12), one O(13), one O(17), one O(3), one O(4), and one O(9) atom to form NiO6 octahedra that share  a cornercorner with one C(1)P2CO tetrahedra,  a cornercorner with one P(1)CO3 tetrahedra,  a cornercorner with one P(2)CO3 tetrahedra,  a cornercorner with one P(3)CO3 tetrahedra,  a cornercorner with one P(4)CO3 tetrahedra, and  an edgeedge with one Ni(3)O6 octahedra. The Ni(2)-O(12) bond length is 2.01 Å. The Ni(2)-O(13) bond length is 2.08 Å. The Ni(2)-O(17) bond length is 2.17 Å. The Ni(2)-O(3) bond length is 2.07 Å. The Ni(2)-O(4) bond length is 2.00 Å. The Ni(2)-O(9) bond length is 2.17 Å. In the third Ni site, Ni(3) is bonded to one O(10), one O(11), one O(14), one O(18), one O(3), and one O(4) atom to form NiO6 octahedra that share  a cornercorner with one C(2)P2CO tetrahedra,  a cornercorner with one P(1)CO3 tetrahedra,  a cornercorner with one P(2)CO3 tetrahedra,  a cornercorner with one P(3)CO3 tetrahedra,  a cornercorner with one P(4)CO3 tetrahedra, and  an edgeedge with one Ni(2)O6 octahedra. The Ni(3)-O(10) bond length is 2.16 Å. The Ni(3)-O(11) bond length is 2.01 Å. The Ni(3)-O(14) bond length is 2.08 Å. The Ni(3)-O(18) bond length is 2.17 Å. The Ni(3)-O(3) bond length is 2.00 Å. The Ni(3)-O(4) bond length is 2.07 Å. There are eleven inequivalent C sites. In the first C site, C(1) is bonded to one C(3), one P(1), one P(3), and one O(13) atom to form distorted CP2CO tetrahedra that share  a cornercorner with one Ni(2)O6 octahedra and  a cornercorner with one O(9)NiPH2 tetrahedra. The corner-sharing octahedral tilt angles are 78°. The C(1)-C(3) bond length is 1.53 Å. The C(1)-P(1) bond length is 1.87 Å. The C(1)-P(3) bond length is 1.87 Å. The C(1)-O(13) bond length is 1.45 Å. In the second C site, C(2) is bonded to one C(4), one P(2), one P(4), and one O(14) atom to form distorted CP2CO tetrahedra that share  a cornercorner with one Ni(3)O6 octahedra and  a cornercorner with one O(10)NiPH2 tetrahedra. The corner-sharing octahedral tilt angles are 78°. The C(2)-C(4) bond length is 1.53 Å. The C(2)-P(2) bond length is 1.87 Å. The C(2)-P(4) bond length is 1.87 Å. The C(2)-O(14) bond length is 1.45 Å. In the third C site, C(3) is bonded in a distorted water-like geometry to one C(1); one C(5,6); one H(13,14); and one H(15,16) atom. The C(3)-C(5,6) bond length is 1.50 Å. The C(3)-H(13,14) bond length is 1.10 Å. The C(3)-H(15,16) bond length is 1.10 Å. In the fourth C site, C(4) is bonded in a distorted water-like geometry to one C(2); one C(5,6); one H(13,14); and one H(15,16) atom. The C(4)-C(5,6) bond length is 1.50 Å. The C(4)-H(13,14) bond length is 1.10 Å. The C(4)-H(15,16) bond length is 1.10 Å. In the fifth C site, C(5,6) is bonded in a trigonal planar geometry to one C(13); one C(3); and one C(7,8) atom. The C(5,6)-C(13) bond length is 1.39 Å. The C(5,6)-C(7,8) bond length is 1.40 Å. In the sixth C site, C(7,8) is bonded in a distorted single-bond geometry to one C(5,6); one C(9,10); and one H(17,18) atom. The C(7,8)-C(9,10) bond length is 1.39 Å. The C(7,8)-H(17,18) bond length is 1.09 Å. In the seventh C site, C(9,10) is bonded in a distorted trigonal planar geometry to one C(11); one C(7,8); and one H(19,20) atom. The C(9,10)-C(11) bond length is 1.39 Å. The C(9,10)-H(19,20) bond length is 1.09 Å. In the eighth C site, C(11) is bonded in a distorted bent 120 degrees geometry to one C(9,10); one N(1); and one H(21,22) atom. The C(11)-N(1) bond length is 1.35 Å. The C(11)-H(21,22) bond length is 1.09 Å. In the ninth C site, C(12) is bonded in a distorted bent 120 degrees geometry to one C(9,10); one N(2); and one H(21,22) atom. The C(12)-C(9,10) bond length is 1.39 Å. The C(12)-N(2) bond length is 1.35 Å. The C(12)-H(21,22) bond length is 1.09 Å. In the tenth C site, C(13) is bonded in a distorted trigonal planar geometry to one C(5,6); one N(1); and one H(23,24) atom. The C(13)-N(1) bond length is 1.35 Å. The C(13)-H(23,24) bond length is 1.09 Å. In the eleventh C site, C(14) is bonded in a distorted trigonal planar geometry to one C(5,6); one N(2); and one H(23,24) atom. The C(14)-C(5,6) bond length is 1.39 Å. The C(14)-N(2) bond length is 1.35 Å. The C(14)-H(23,24) bond length is 1.09 Å. There are four inequivalent P sites. In the first P site, P(1) is bonded to one C(1), one O(1), one O(3), and one O(5) atom to form distorted PCO3 tetrahedra that share  a cornercorner with one Ni(1)O6 octahedra,  a cornercorner with one Ni(2)O6 octahedra,  a cornercorner with one Ni(3)O6 octahedra, and  a cornercorner with one P(3)CO3 tetrahedra. The corner-sharing octahedral tilt angles range from 27-69°. The P(1)-O(1) bond length is 1.52 Å. The P(1)-O(3) bond length is 1.56 Å. The P(1)-O(5) bond length is 1.53 Å. In the second P site, P(2) is bonded to one C(2), one O(2), one O(4), and one O(6) atom to form distorted PCO3 tetrahedra that share  a cornercorner with one Ni(1)O6 octahedra,  a cornercorner with one Ni(2)O6 octahedra,  a cornercorner with one Ni(3)O6 octahedra, and  a cornercorner with one P(4)CO3 tetrahedra. The corner-sharing octahedral tilt angles range from 27-69°. The P(2)-O(2) bond length is 1.52 Å. The P(2)-O(4) bond length is 1.56 Å. The P(2)-O(6) bond length is 1.53 Å. In the third P site, P(3) is bonded to one C(1), one O(11), one O(7), and one O(9) atom to form PCO3 tetrahedra that share  a cornercorner with one Ni(1)O6 octahedra,  a cornercorner with one Ni(2)O6 octahedra,  a cornercorner with one Ni(3)O6 octahedra, and  a cornercorner with one P(1)CO3 tetrahedra. The corner-sharing octahedral tilt angles range from 43-70°. The P(3)-O(11) bond length is 1.54 Å. The P(3)-O(7) bond length is 1.51 Å. The P(3)-O(9) bond length is 1.58 Å. In the fourth P site, P(4) is bonded to one C(2), one O(10), one O(12), and one O(8) atom to form PCO3 tetrahedra that share  a cornercorner with one Ni(1)O6 octahedra,  a cornercorner with one Ni(2)O6 octahedra,  a cornercorner with one Ni(3)O6 octahedra, and  a cornercorner with one P(2)CO3 tetrahedra. The corner-sharing octahedral tilt angles range from 43-70°. The P(4)-O(10) bond length is 1.58 Å. The P(4)-O(12) bond length is 1.54 Å. The P(4)-O(8) bond length is 1.51 Å. There are two inequivalent N sites. In the first N site, N(1) is bonded in a trigonal planar geometry to one C(11), one C(13), and one H(11) atom. The N(1)-H(11) bond length is 1.07 Å. In the second N site, N(2) is bonded in a trigonal planar geometry to one C(12), one C(14), and one H(12) atom. The N(2)-H(12) bond length is 1.07 Å. There are eighteen inequivalent H sites. In the first H site, H(1) is bonded in a distorted linear geometry to one O(10) and one O(13) atom. The H(1)-O(10) bond length is 1.52 Å. The H(1)-O(13) bond length is 1.03 Å. In the second H site, H(2) is bonded in a distorted linear geometry to one O(14) and one O(9) atom. The H(2)-O(14) bond length is 1.03 Å. The H(2)-O(9) bond length is 1.52 Å. In the third H site, H(3) is bonded in a single-bond geometry to one O(12) and one O(15) atom. The H(3)-O(12) bond length is 1.75 Å. The H(3)-O(15) bond length is 1.00 Å. In the fourth H site, H(4) is bonded in a single-bond geometry to one O(11) and one O(16) atom. The H(4)-O(11) bond length is 1.75 Å. The H(4)-O(16) bond length is 1.00 Å. In the fifth H site, H(5) is bonded in a single-bond geometry to one O(15) atom. The H(5)-O(15) bond length is 0.98 Å. In the sixth H site, H(6) is bonded in a single-bond geometry to one O(16) atom. The H(6)-O(16) bond length is 0.98 Å. In the seventh H site, H(7) is bonded in a single-bond geometry to one O(10) and one O(17) atom. The H(7)-O(10) bond length is 1.72 Å. The H(7)-O(17) bond length is 1.01 Å. In the eighth H site, H(8) is bonded in a single-bond geometry to one O(18) and one O(9) atom. The H(8)-O(18) bond length is 1.01 Å. The H(8)-O(9) bond length is 1.71 Å. In the ninth H site, H(9) is bonded in a single-bond geometry to one O(17) atom. The H(9)-O(17) bond length is 0.99 Å. In the tenth H site, H(10) is bonded in a single-bond geometry to one O(18) atom. The H(10)-O(18) bond length is 0.99 Å. In the eleventh H site, H(11) is bonded in a distorted single-bond geometry to one N(1) and one O(6) atom. The H(11)-O(6) bond length is 1.68 Å. In the twelfth H site, H(12) is bonded in a distorted single-bond geometry to one N(2) and one O(5) atom. The H(12)-O(5) bond length is 1.69 Å. In the thirteenth H site, H(13,14) is bonded in a single-bond geometry to one C(3) atom. In the fourteenth H site, H(15,16) is bonded in a single-bond geometry to one C(3) atom. In the fifteenth H site, H(17,18) is bonded in a single-bond geometry to one C(7,8) atom. In the sixteenth H site, H(19,20) is bonded in a single-bond geometry to one C(9,10) atom. In the seventeenth H site, H(21,22) is bonded in a single-bond geometry to one C(11) atom. In the eighteenth H site, H(23,24) is bonded in a single-bond geometry to one C(13) atom. There are eighteen inequivalent O sites. In the first O site, O(1) is bonded in a bent 120 degrees geometry to one Ni(1) and one P(1) atom. In the second O site, O(2) is bonded in a bent 120 degrees geometry to one Ni(1) and one P(2) atom. In the third O site, O(3) is bonded in a distorted T-shaped geometry to one Ni(2), one Ni(3), and one P(1) atom. In the fourth O site, O(4) is bonded in a distorted T-shaped geometry to one Ni(2), one Ni(3), and one P(2) atom. In the fifth O site, O(5) is bonded in a distorted water-like geometry to one P(1) and one H(12) atom. In the sixth O site, O(6) is bonded in a distorted water-like geometry to one P(2) and one H(11) atom. In the seventh O site, O(7) is bonded in a distorted bent 150 degrees geometry to one Ni(1) and one P(3) atom. In the eighth O site, O(8) is bonded in a distorted bent 150 degrees geometry to one Ni(1) and one P(4) atom. In the ninth O site, O(9) is bonded to one Ni(2), one P(3), one H(2), and one H(8) atom to form distorted ONiPH2 tetrahedra that share  a cornercorner with one C(1)P2CO tetrahedra. In the tenth O site, O(10) is bonded to one Ni(3), one P(4), one H(1), and one H(7) atom to form distorted ONiPH2 tetrahedra that share  a cornercorner with one C(2)P2CO tetrahedra. In the eleventh O site, O(11) is bonded in a 3-coordinate geometry to one Ni(3), one P(3), and one H(4) atom. In the twelfth O site, O(12) is bonded in a 3-coordinate geometry to one Ni(2), one P(4), and one H(3) atom. In the thirteenth O site, O(13) is bonded in a 3-coordinate geometry to one Ni(2), one C(1), and one H(1) atom. In the fourteenth O site, O(14) is bonded in a 3-coordinate geometry to one Ni(3), one C(2), and one H(2) atom. In the fifteenth O site, O(15) is bonded in a distorted water-like geometry to one Ni(1), one H(3), and one H(5) atom. In the sixteenth O site, O(16) is bonded in a distorted water-like geometry to one Ni(1), one H(4), and one H(6) atom. In the seventeenth O site, O(17) is bonded in a distorted water-like geometry to one Ni(2), one H(7), and one H(9) atom. In the eighteenth O site, O(18) is bonded in a distorted water-like geometry to one Ni(3), one H(10), and one H(8) atom. Linkers: 2 [O]P([O])(=O)C(O)(CC1=CN[CH]C=C1)P([O])([O])=O. Metal clusters: 3 [Ni]. The MOF has largest included sphere 2.93 A, density 2.05 g/cm3, surface area 2880.01 m2/g, accessible volume 0.15 cm3/g