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Synthesis and Characterization of New Ce(IV)-MOFs Exhibiting Various Framework Topologies

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We report on the applicability of an easy general synthesis procedure for the formation of Ce(W)-MOFs which contain hexanuclear clusters. Thus, the series of Ce(IV)-based MOFs isoreticular to their Zr analogues has been extended to reo and spn topologies. Four new MOFs denoted as Ce-UiO-66-BPyDC Ce-6(mu(3)-O)(4)(mu-OH)(4)(BPyDC)(6) (BPyDC2- = 2,2'-bipyridine-5,5'-dicarbox-ylate), Ce-DUT-67-PZDC Ce-6(mu-O)(4)(mu(3)-OH)(4)(PZDC)(4)(OH)(4)(H2O)(4) (PZDC(2-) = 3,5-pyrazole-dicarboxylate), Ce-DUT-67-TDC Ce-6(mu(3)-O)(4)(mu 0OH)(4)(TDC)(4)(OH)(4)(H2O)(4) (TDC2- = 2,5-thiophenedicarboxylate), and Ce-MOF-808 Ce-6(mu(3)-O)(4)(mu(3)-OH)(4)(BTC)(2)(OH)(6) (H2O)(6) (BTC3- = benzene-1,3,5-tricarboxylate) were obtained under mild reaction conditions (100 degrees C) and after short reaction times (15 min) using a modulated synthesis approach. The MOFs differ in their connectivity of the Ce6O4(OH)(4)(-CO2)x (x = 12, 8, 6) cluster, the geometry of the organic linker molecules (linear and bent dicarboxylic acids, tricarboxylic acid), and the resulting topology (fcu, reo, spn). The structures of all Ce-MOFs were confirmed using PXRD data by Rietveld refinement and Le Bail fitting. The heterocyclic aromatic dicarboxylic acids H2PZDC and H2TDC lead to MOFs which are both isostructural to DUT-67 due to the similar linker geometries. Ce-UiO-66-BPyDC and Ce-MOF-808 are thermally stable up to 330 and 150 degrees C, respectively, as proven by VTPXRD measurements. N-2 sorption experiments reveal large specific surface areas of 2120 m(2) g(-1) for Ce-UiO-66-BPyDC and 1725 m(2) g(-1) for Ce-MOF-808.

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