“Fluoride molecular scissors”: A rational construction of new Mo(VI) oxofluorido/1,2,4-triazole MOFs

Senchyk, Ganna A.; Lysenko, Andrey B.; Krautscheid, Harald; Domasevitch, Konstantin V.

doi:10.1016/j.inoche.2011.05.022

Cited by 14 publications

(7 citation statements)

References 32 publications

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“…1,3-Diaminoadamantane ( 6 ), Ad-(NH 2 ) 2 , was prepared from 1,3-dibromoadamantane (28% yield) following a reported method . The related compound BAd-(NH 2 ) 2 7 was obtained from BAd, which was itself prepared from 1-bromoadamantane homocoupling by metallic sodium. , From commercial diamantane, DAd-(NH 2 ) 2 8 was obtained after selective dibromination of 4,9-C–H apical positions . Ad-COOH 1 and Ad-(COOH) 2 2 are commercially available, and DAd-(COOH) 2 4 was prepared based on literature methods and isolated (23% yield) starting from 4,9-dihydroxy-diamantane. , BAd-(COOH) 2 3 was also synthesized; however, its insolubility in common organic solvents obviated its use as a stabilizer of Ru NPs.…”

Section: Resultsmentioning

confidence: 99%

“…40 The related compound BAd-(NH 2 ) 2 7 was obtained from BAd, which was itself prepared from 1-bromoadamantane homocoupling by metallic sodium. 40,41 From commercial diamantane, DAd-(NH 2 ) 2 8 was obtained after selective dibromination of 4,9-C−H apical positions. 42 Ad-COOH 1 and Ad-(COOH) 2 2 are commercially available, and DAd-(COOH) 2 4 was prepared based on literature methods and isolated (23% yield) starting from 4,9-dihydroxy-diamantane.…”

Section: ■ Resultsmentioning

confidence: 99%

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3D Ruthenium Nanoparticle Covalent Assemblies from Polymantane Ligands for Confined Catalysis

et al. 2020

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The synthesis of metal nanoparticle (NP) assemblies stabilized by functional molecules is an important research topic in nanoscience, and the ability to control interparticle distances and positions in NP assemblies is one of the major challenges in designing and understanding functional nanostructures. Here, two series of functionalized adamantanes, bisadamantanes and diamantanes bearing carboxylic acid or amine functional groups have been used as building blocks to produce, via a straightforward method, networks of ruthenium NP. Both the nature of the ligand and the Ru/ligand ratio affect the interparticle distance in the assemblies. The use of 1,3-adamantanedicarboxylic acid allows the synthesis of 3D networks of 1.7-1.9 nm Ru NP presenting interparticle distance of 2.5-2.7 nm. The surface interaction between Ru NP and the ligands were investigated spectroscopically using a 13 C labeled ligand, as well as theoretically with Density Functional Theory (DFT) calculations. We found that Ru species formed during the NP assembly are able to partially decarbonylate carboxylic acid ligands at room temperature. Decarbonylation of a carboxylic acid at room temperature in the presence of dihydrogen usually occurs on catalysts at much higher temperature and pressure. This result reveals a very high reactivity of ruthenium species formed during network assembling. The Ru NP networks were found active catalysts for the selective hydrogenation of phenyl acetylene, reaching good selectivity towards styrene. Overall, we demonstrated that catalyst activity, selectivity, and NP network stability are significantly affected by Ru NP interparticle distance, and electronic ligand effects. As such, these materials constitute a unique set that should allow a better understanding of the complex surface chemistry in carbonsupported metal catalysts.

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Section: Resultsmentioning

confidence: 99%

Section: ■ Resultsmentioning

confidence: 99%

3D Ruthenium Nanoparticle Covalent Assemblies from Polymantane Ligands for Confined Catalysis

et al. 2020

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“…The tr 2 pr ligand contains a linear aliphatic -(CH 2 ) 3 - spacer between tr-termini suggesting the existence of conformational flexibility similar to that described for the glutarate anion: anti – anti , anti – gauche , and gauche – gauche . In 1 , tr 2 pr adopts an anti – anti conformation type that provides a 10.733(1) Å distance for the interconnection between the dinuclear [Mo 2 F 2 O 5 (tr) 2 ] units, predetermining a more favorable 1D zigzag motif, running along the a axis.…”

Section: Crystal Structuresmentioning

confidence: 99%

Unprecedented Trapping of Difluorooctamolybdate Anions within an α-Polonium Type Coordination Network

et al. 2013

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New fluorinated hybrid solids [Mo2F2O5(tr2pr)] (1), [Co3(tr2pr)2(MoO4)2F2]·7H2O (2), and [Co3(H2O)2(tr2pr)3(Mo8O26F2)]·3H2O (3) (tr2pr = 1,3-bis(1,2,4-triazol-4-yl)propane) were prepared from the reaction systems consisting of Co(OAc)2/CoF2 and MoO3/(NH4)6Mo7O24, as Co(II) and Mo(VI) sources, in water (2) or in aqueous HF (1, 3) employing mild hydrothermal conditions. The tr2pr ligand serves as a conformationally flexible tetradentate donor. In complex 1, the octahedrally coordinated Mo atoms are linked in the discrete corner-sharing {Mo2(μ2-O)F2O4N4} unit in which a pair of tr-heterocycles (tr = 1,2,4-triazole) is arranged in cis-positions opposite to "molybdenyl" oxygen atoms. The anti-anti conformation type of tr2pr facilitates the tight zigzag chain packing motif. The crystal structure of the mixed-anion complex salt 2 consists of trinuclear [Co3(μ3-MoO4)2(μ2-F)2] units self-assembling in Co(II)-undulating chains (Co···Co 3.0709(15) and 3.3596(7) Å), which are cross-linked by tr2pr in layers. In 3, containing condensed oxyfluoromolybdate species, linear centrosymmetric [Co3(μ2-tr)6](6+) SBUs are organized at distances of 10.72-12.45 Å in an α-Po-like network using bitopic tr-linkers. The octahedral {N6} and {N3O3} environments of the central and peripheral cobalt atoms, respectively, are filled by triazole N atoms, water molecules, and coordinating [Mo8O26F2](6-) anions. Acting as a tetradentate O-donor, each difluorooctamolybdate anion anchors four [Co3(μ2-tr)6](6+) units through their peripheral Co-sites, which consequently leads to a novel type of a two-nodal 4,10-c net with the Schläfli symbol {3(2).4(3).5}{3(4).4(20).5(16).6(5)}. The 2D and 3D coordination networks of 2 and 3, respectively, are characterized by significant overall antiferromagnetic exchange interactions (J/k) between the Co(II) spin centers on the order of -8 and -4 K. The [Mo8O26F2](6-) anion is investigated in detail by quantum chemical calculations.

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“…Coordination polymers and metal-organic frameworks in particular are promising materials with a wide range of potential applications-gas storage and separation [11,12], enantioselective catalysis [13,14], supramolecular systems design [15], pollutant sensing [16,17], water purification [18], fabrication of electrochemical devices [19,20], and biological activity [21]. Coordination polymers based on 1,3-bis(1,2,4-triazol-4-yl)adamantane with Mo(IV), Cu(II), Zn(II), Cd(II), Ag(I), bimetallic Ag(I)/V(V), and Cu(II)/Mo(IV) were successfully synthesized and characterized by Domasevitch research group [22][23][24][25][26][27][28][29][30][31], but the coordination chemistry of its isomer, 1,3-bis(1,2,4-triazol-1-yl)adamantane remained unexplored.…”

Section: Introductionmentioning

confidence: 99%

Synthesis, Crystal Structure, and Luminescence of Cadmium(II) and Silver(I) Coordination Polymers Based on 1,3-Bis(1,2,4-triazol-1-yl)adamantane

et al. 2021

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Coordination polymers with a new rigid ligand 1,3-bis(1,2,4-triazol-1-yl)adamantane (L) were prepared by its reaction with cadmium(II) or silver(I) nitrates. Crystal structure of the coordination polymers was determined using single-crystal X-ray diffraction analysis. Silver formed two-dimensional coordination polymer [Ag(L)NO3]n, in which metal ions are linked by 1,3-bis(1,2,4-triazol-1-yl)adamantane ligands, coordinated by nitrogen atoms at positions 2 and 4 of 1,2,4-triazole rings. Layers of the coordination polymer consist of rare 18- and 30-membered {Ag2L2} and {Ag4L4} metallocycles. Cadmium(II) nitrate formed two kinds of one-dimensional coordination polymers depending on the metal-to-ligand ratio used in the synthesis. Coordination polymer [Cd(L)2(NO3)2]n was obtained in case of a 1:2 M:L ratio, while for M:L = 2:1 product {[Cd(L)(NO3)2(CH3OH)]·0.5CH3OH}n was isolated. All coordination polymers demonstrated ligand-centered emission near 450 nm upon excitation at 370 nm.

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“Fluoride molecular scissors”: A rational construction of new Mo(VI) oxofluorido/1,2,4-triazole MOFs

Cited by 14 publications

References 32 publications

3D Ruthenium Nanoparticle Covalent Assemblies from Polymantane Ligands for Confined Catalysis

3D Ruthenium Nanoparticle Covalent Assemblies from Polymantane Ligands for Confined Catalysis

Unprecedented Trapping of Difluorooctamolybdate Anions within an α-Polonium Type Coordination Network

Synthesis, Crystal Structure, and Luminescence of Cadmium(II) and Silver(I) Coordination Polymers Based on 1,3-Bis(1,2,4-triazol-1-yl)adamantane

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