Preparation, Structures, and Photocatalytic Properties of Three New Uranyl−Organic Assembly Compounds

Abstract

Three new uranyl-organic coordination polymers (UO2)8(NDC)12(4,4'-bipyH2)3(4,4'-bipyH)3 (1), (UO2)3O[Ag(2,2'-bipy)2]2(NDC)3 (2), and (UO2)2(NDC)2(2,2'-bipy)2 (3), where NDC=1,4-naphthalenedicarboxylate and bipy=bipyridine, have been prepared in hydrothermal conditions. Both 1 and 2 possess a 2D structure while 3 is composed of 1D zigzag chains. In 1 there are mononuclear pentagonal-bipyramidal U-O polyhedra and 1D channels filled with 4,4'-bipy molecules, whereas in 2 there are mononuclear hexagonal-bipyramidal U-O polyhedra and tetranuclear pentagonal-bipyramidal U-O clusters which form 2D channels with occluded [Ag(2,2'-bipy)2]+ counterions. In 3 both the NDC and the bipy ligands coordinate to uranyl centers, leading to hexagonal-bipyramidal polyhedra which are connected to form 1D zigzag chains. Under UV or visible irradiation, 1 and 2 degrade rhodamine B with similar efficiency. The correlation between photocatalytic reaction rate and oxygen concentration for 1 and 2 has also been elucidated. Crystal data: 1, triclinic, space group P1, a=11.037(2) A, b=15.126(3) A, c=15.660(3) A, alpha=62.05(3) degrees, beta=72.26(3) degrees, gamma=82.05(3) degrees, and Z=2; 2, triclinic, space group P1, a=14.161(3) A, b=15.122(3) A, c=18.212(4) A, alpha=85.73(3) degrees, beta=76.99(3) degrees, gamma=67.32(3) degrees, and Z=2; 3, monoclinic, space group P2(1)/n, a=10.7976(18) A, b=31.501(6) A, c=11.590(2) A, beta=97.609(4) degrees, and Z=4.

Structures and photocatalytic activities of metal-organic frameworks derived from rigid aromatic dicarboxylate acids and flexible imidazole-based linkers

“…3 and 4, Figs.S4 and S5). Obviously, the X3B is degraded about 60 and 80% in the presence of 1 and 2 after 9 h irradiation, which is comparable with those of the reported uranyl-organic assembly compounds [17]. In addition, the number of moles for degradated X3B per gram metal atom in the presence of 1 and 2 is 6.64 × 10 − 6 and 16.61 × 10 − 6 mol/g, respectively (Fig.…”

“…Nowadays, much effort has also been devoted to developing new photocatalytic materials based on metal-organic frameworks, which is motivated largely by a demand for solving pollution problems in view of their potential applications in the green degradation of organic pollutants [16][17][18][19][20][21][22][23].…”

Syntheses, crystal structures and properties of three novel coordination polymers with tripodal imidazole-containing ligands and benzenetetracarboxylate

“…Novel coordination polymers with intriguing structures and interesting properties have been designed and synthesized, where flexible bis(imidazole) ligands together with multi-carboxylate have been widely used in the construction of multi-dimensional frameworks as both of them adopt a variety of coordination modes to satisfy the coordination geometric requirements of the central metal ions [1][2][3][4][5][6][7]. However, coordination polymers with rigid imidazole-containing ligands and multi-carboxylate as mixed ligands are less documented [8][9][10][11].…”

Nanomaterials and nanotechnologies in nuclear energy chemistry

“…However, in the strict sense, this material is just a uranium-inorganic framework material based on an organic template. To date, a series of uranyl-organic materials including 1-D chains, 2-D layers, and 3-D frameworks have been synthesized [23][24][25][26][27][28][29][30][31][32][33][34][35][36][37][38][39][40][41][42] In China, the UOF (uranium organic-framework) materials have also been extensively studied [38][39][40][41][42]. Chen et al have prepared a series of UOF materials under hydrothermal conditions.…”