U14(SO4)19 crystallizes in the tetragonal I4/m space group. There are four inequivalent U sites. In the first U site, U(1) is bonded in a pentagonal planar geometry to one O(1), one O(12), one O(13), one O(5), and one O(7) atom. The U(1)-O(1) bond length is 2.45 Å. The U(1)-O(12) bond length is 2.38 Å. The U(1)-O(13) bond length is 2.38 Å. The U(1)-O(5) bond length is 2.41 Å. The U(1)-O(7) bond length is 2.36 Å. In the second U site, U(2) is bonded in a pentagonal planar geometry to one O(14), one O(15), one O(16), one O(4), and one O(6) atom. The U(2)-O(14) bond length is 2.39 Å. The U(2)-O(15) bond length is 2.38 Å. The U(2)-O(16) bond length is 2.40 Å. The U(2)-O(4) bond length is 2.47 Å. The U(2)-O(6) bond length is 2.37 Å. In the third U site, U(3) is bonded in a 4-coordinate geometry to one O(11), one O(18), one O(2), and one O(9) atom. The U(3)-O(11) bond length is 2.39 Å. The U(3)-O(18) bond length is 2.40 Å. The U(3)-O(2) bond length is 2.43 Å. The U(3)-O(9) bond length is 2.35 Å. In the fourth U site, U(4) is bonded in a pentagonal planar geometry to one O(19), two equivalent O(10), and two equivalent O(3) atoms. The U(4)-O(19) bond length is 2.30 Å. Both U(4)-O(10) bond lengths are 2.36 Å. Both U(4)-O(3) bond lengths are 2.42 Å. There are six inequivalent S sites. In the first S site, S(1) is bonded in a tetrahedral geometry to one O(12), one O(16), one O(3), and one O(5) atom. The S(1)-O(12) bond length is 1.45 Å. The S(1)-O(16) bond length is 1.45 Å. The S(1)-O(3) bond length is 1.46 Å. The S(1)-O(5) bond length is 1.48 Å. In the second S site, S(2) is bonded in a tetrahedral geometry to one O(10), one O(2), one O(4), and one O(7) atom. The S(2)-O(10) bond length is 1.47 Å. The S(2)-O(2) bond length is 1.48 Å. The S(2)-O(4) bond length is 1.47 Å. The S(2)-O(7) bond length is 1.47 Å. In the third S site, S(3) is bonded in a tetrahedral geometry to one O(13), one O(15), one O(8), and one O(9) atom. The S(3)-O(13) bond length is 1.48 Å. The S(3)-O(15) bond length is 1.46 Å. The S(3)-O(8) bond length is 1.44 Å. The S(3)-O(9) bond length is 1.48 Å. In the fourth S site, S(4) is bonded in a tetrahedral geometry to one O(11), one O(14), one O(17), and one O(6) atom. The S(4)-O(11) bond length is 1.47 Å. The S(4)-O(14) bond length is 1.48 Å. The S(4)-O(17) bond length is 1.42 Å. The S(4)-O(6) bond length is 1.47 Å. In the fifth S site, S(5) is bonded in a tetrahedral geometry to one O(19), one O(20), and two equivalent O(18) atoms. The S(5)-O(19) bond length is 1.37 Å. The S(5)-O(20) bond length is 1.41 Å. Both S(5)-O(18) bond lengths are 1.42 Å. In the sixth S site, S(6) is bonded in a tetrahedral geometry to four equivalent O(1) atoms. All S(6)-O(1) bond lengths are 1.47 Å. There are twenty inequivalent O sites. In the first O site, O(1) is bonded in a single-bond geometry to one U(1) and one S(6) atom. In the second O site, O(2) is bonded in a single-bond geometry to one U(3) and one S(2) atom. In the third O site, O(3) is bonded in a distorted single-bond geometry to one U(4) and one S(1) atom. In the fourth O site, O(4) is bonded in a distorted single-bond geometry to one U(2) and one S(2) atom. In the fifth O site, O(5) is bonded in a distorted single-bond geometry to one U(1) and one S(1) atom. In the sixth O site, O(6) is bonded in a distorted bent 150 degrees geometry to one U(2) and one S(4) atom. In the seventh O site, O(7) is bonded in a distorted single-bond geometry to one U(1) and one S(2) atom. In the eighth O site, O(8) is bonded in a single-bond geometry to one S(3) atom. In the ninth O site, O(9) is bonded in a single-bond geometry to one U(3) and one S(3) atom. In the tenth O site, O(10) is bonded in a distorted single-bond geometry to one U(4) and one S(2) atom. In the eleventh O site, O(11) is bonded in a distorted single-bond geometry to one U(3) and one S(4) atom. In the twelfth O site, O(12) is bonded in a distorted single-bond geometry to one U(1) and one S(1) atom. In the thirteenth O site, O(13) is bonded in a single-bond geometry to one U(1) and one S(3) atom. In the fourteenth O site, O(14) is bonded in a distorted single-bond geometry to one U(2) and one S(4) atom. In the fifteenth O site, O(15) is bonded in a distorted bent 150 degrees geometry to one U(2) and one S(3) atom. In the sixteenth O site, O(16) is bonded in a distorted single-bond geometry to one U(2) and one S(1) atom. In the seventeenth O site, O(17) is bonded in a single-bond geometry to one S(4) atom. In the eighteenth O site, O(18) is bonded in a single-bond geometry to one U(3) and one S(5) atom. In the nineteenth O site, O(19) is bonded in a distorted single-bond geometry to one U(4) and one S(5) atom. In the twentieth O site, O(20) is bonded in a single-bond geometry to one S(5) atom. Linkers: 76 [O]S([O])(=O)=O. Metal clusters: 56 [U]. The MOF has largest included sphere 12.37 A, density 2.22 g/cm3, surface area 1560.66 m2/g, accessible volume 0.29 cm3/g