PuCP2H4O7 crystallizes in the triclinic P-1 space group. There are two inequivalent Pu sites. In the first Pu site, Pu(1) is bonded in a 7-coordinate geometry to one O(10), one O(11), one O(13), one O(2), one O(3), one O(5), and one O(7) atom. The Pu(1)-O(10) bond length is 2.23 Å. The Pu(1)-O(11) bond length is 2.67 Å. The Pu(1)-O(13) bond length is 2.31 Å. The Pu(1)-O(2) bond length is 2.26 Å. The Pu(1)-O(3) bond length is 2.22 Å. The Pu(1)-O(5) bond length is 2.24 Å. The Pu(1)-O(7) bond length is 2.21 Å. In the second Pu site, Pu(2) is bonded in a 7-coordinate geometry to one O(1), one O(12), one O(14), one O(4), one O(6), one O(8), and one O(9) atom. The Pu(2)-O(1) bond length is 2.26 Å. The Pu(2)-O(12) bond length is 2.67 Å. The Pu(2)-O(14) bond length is 2.31 Å. The Pu(2)-O(4) bond length is 2.22 Å. The Pu(2)-O(6) bond length is 2.24 Å. The Pu(2)-O(8) bond length is 2.22 Å. The Pu(2)-O(9) bond length is 2.23 Å. There are two inequivalent C sites. In the first C site, C(1) is bonded in a distorted tetrahedral geometry to one P(1), one P(3), one H(1), and one H(3) atom. The C(1)-P(1) bond length is 1.81 Å. The C(1)-P(3) bond length is 1.81 Å. The C(1)-H(1) bond length is 1.10 Å. The C(1)-H(3) bond length is 1.10 Å. In the second C site, C(2) is bonded in a distorted tetrahedral geometry to one P(2), one P(4), one H(2), and one H(4) atom. The C(2)-P(2) bond length is 1.81 Å. The C(2)-P(4) bond length is 1.81 Å. The C(2)-H(2) bond length is 1.10 Å. The C(2)-H(4) bond length is 1.10 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(7), and one O(9) atom to form corner-sharing PCO3 tetrahedra. The P(1)-O(1) bond length is 1.54 Å. The P(1)-O(7) bond length is 1.54 Å. The P(1)-O(9) bond length is 1.54 Å. In the second P site, P(2) is bonded to one C(2), one O(10), one O(2), and one O(8) atom to form corner-sharing PCO3 tetrahedra. The P(2)-O(10) bond length is 1.54 Å. The P(2)-O(2) bond length is 1.54 Å. The P(2)-O(8) bond length is 1.54 Å. In the third P site, P(3) is bonded to one C(1), one O(13), one O(3), and one O(5) atom to form corner-sharing PCO3 tetrahedra. The P(3)-O(13) bond length is 1.53 Å. The P(3)-O(3) bond length is 1.55 Å. The P(3)-O(5) bond length is 1.55 Å. In the fourth P site, P(4) is bonded to one C(2), one O(14), one O(4), and one O(6) atom to form corner-sharing PCO3 tetrahedra. The P(4)-O(14) bond length is 1.53 Å. The P(4)-O(4) bond length is 1.55 Å. The P(4)-O(6) bond length is 1.55 Å. There are seven 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(1) atom. In the fourth H site, H(4) is bonded in a single-bond geometry to one C(2) atom. In the fifth H site, H(5) is bonded in a single-bond geometry to one O(11) atom. The H(5)-O(11) bond length is 0.97 Å. In the sixth H site, H(6) is bonded in a single-bond geometry to one O(12) atom. The H(6)-O(12) bond length is 0.97 Å. In the seventh H site, H(7,8) is bonded in a single-bond geometry to one O(11) atom. The H(7,8)-O(11) bond length is 0.98 Å. There are fourteen inequivalent O sites. In the first O site, O(1) is bonded in a distorted bent 150 degrees geometry to one Pu(2) and one P(1) atom. In the second O site, O(2) is bonded in a distorted bent 150 degrees geometry to one Pu(1) and one P(2) atom. In the third O site, O(3) is bonded in a distorted bent 150 degrees geometry to one Pu(1) and one P(3) atom. In the fourth O site, O(4) is bonded in a distorted bent 150 degrees geometry to one Pu(2) and one P(4) atom. In the fifth O site, O(5) is bonded in a distorted bent 120 degrees geometry to one Pu(1) and one P(3) atom. In the sixth O site, O(6) is bonded in a distorted bent 120 degrees geometry to one Pu(2) and one P(4) atom. In the seventh O site, O(7) is bonded in a distorted bent 150 degrees geometry to one Pu(1) and one P(1) atom. In the eighth O site, O(8) is bonded in a distorted bent 150 degrees geometry to one Pu(2) and one P(2) atom. In the ninth O site, O(9) is bonded in a bent 150 degrees geometry to one Pu(2) and one P(1) atom. In the tenth O site, O(10) is bonded in a bent 150 degrees geometry to one Pu(1) and one P(2) atom. In the eleventh O site, O(11) is bonded in a water-like geometry to one Pu(1); one H(5); and one H(7,8) atom. In the twelfth O site, O(12) is bonded in a water-like geometry to one Pu(2); one H(6); and one H(7,8) atom. The O(12)-H(7,8) bond length is 0.98 Å. In the thirteenth O site, O(13) is bonded in a 2-coordinate geometry to one Pu(1) and one P(3) atom. In the fourteenth O site, O(14) is bonded in a 2-coordinate geometry to one Pu(2) and one P(4) atom. Linkers: 4 [O]P([O])(=O)CP([O])([O])=O. Metal clusters: 4 [Pu]. RCSR code: fes. The MOF has largest included sphere 2.47 A, density 4.05 g/cm3, surface area 1600.25 m2/g, accessible volume 0.05 cm3/g