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| Hauptseite > Publikationsdatenbank > Molecular Characteristics of a Mixed-Valence Polyoxovanadate {V IV/V 18 O 42 } in Solution and at the Liquid–Surface Interface > print |
| Hauptseite > Publikationsdatenbank > Molecular Characteristics of a Mixed-Valence Polyoxovanadate {V IV/V 18 O 42 } in Solution and at the Liquid–Surface Interface > print |
| 001 | 830302 | ||
| 005 | 20250129094247.0 | ||
| 024 | 7 | _ | |a 10.1021/acs.jpcc.7b02138 |2 doi |
| 024 | 7 | _ | |a 1932-7447 |2 ISSN |
| 024 | 7 | _ | |a 1932-7455 |2 ISSN |
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| 037 | _ | _ | |a FZJ-2017-03870 |
| 082 | _ | _ | |a 540 |
| 100 | 1 | _ | |a Linnenberg, Oliver |0 P:(DE-HGF)0 |b 0 |
| 245 | _ | _ | |a Molecular Characteristics of a Mixed-Valence Polyoxovanadate {V IV/V 18 O 42 } in Solution and at the Liquid–Surface Interface |
| 260 | _ | _ | |a Washington, DC |c 2017 |b Soc. |
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| 520 | _ | _ | |a The understanding of the molecular state of vanadium-oxo clusters (polyoxovanadates, POVs) in solution and on surface is a key to their target application in catalysis as well as molecular electronics and spintronics. We here report the results of a combined experimental and computational study of the behavior of nucleophilic polyoxoanions [VIV10VV8O42(I)]5– charged balanced by Et4N+ in water, in a one-phase organic solution of N,N-dimethylformamid (DMF) or acetonitrile (MeCN), in a mixed solution of MeCN–water, and at the hybrid liquid–surface interface. The molecular characteristics of the compound (NEt4)5[V18O42(I)] (1) in the given environments were studied by microspectroscopic, electrochemical, scattering, and molecular mechanics methods. Contrary to the situation in pure water, where we observe great agglomeration with a number of intercalated H2O molecules between POVs that are surrounded by the Et4N+ ions, no or only minor agglomeration of redox-active POVs in an unprecedented cation-mediated fashion was detected in pure DMF and MeCN, respectively. An inclusion of 1% water in the MeCN solution does not have an effect significant enough to reinforce agglomeration; however, this leads to the POV···POV interface characterized by the presence of the Et4N+ ions and a small number of H2O molecules. Water amounts of ≥5% trigger the formation of higher oligomers. The deposition of compound 1 from MeCN onto an Au(111) surface affords nearly round-shaped particles (∼10 nm). The use of DMF instead of MeCN results in bigger, irregularly shaped particles (∼30 nm). This change of solvent gives rise to more extensive intermolecular interactions between polyoxoanions and their countercations as well as weaker binding of ion-pairing induced agglomerates to the metallic substrate. Lower concentration of adsorbed molecules leads to a submonolayer coverage and an accompanied change of the POV’s redox state, whereas their higher concentration results in a multilayer coverage that offers the pristine mixed-valence structure of the polyoxoanion. Our study provides first important insights into the reactivity peculiarities of this redox-responsive material class on a solid support. |
| 536 | _ | _ | |a 144 - Controlling Collective States (POF3-144) |0 G:(DE-HGF)POF3-144 |c POF3-144 |f POF III |x 0 |
| 536 | _ | _ | |a 524 - Controlling Collective States (POF3-524) |0 G:(DE-HGF)POF3-524 |c POF3-524 |f POF III |x 1 |
| 536 | _ | _ | |a 6212 - Quantum Condensed Matter: Magnetism, Superconductivity (POF3-621) |0 G:(DE-HGF)POF3-6212 |c POF3-621 |f POF III |x 2 |
| 536 | _ | _ | |a 6213 - Materials and Processes for Energy and Transport Technologies (POF3-621) |0 G:(DE-HGF)POF3-6213 |c POF3-621 |f POF III |x 3 |
| 588 | _ | _ | |a Dataset connected to CrossRef |
| 700 | 1 | _ | |a Moors, Marco |0 P:(DE-Juel1)145323 |b 1 |
| 700 | 1 | _ | |a Solé-Daura, Albert |0 P:(DE-HGF)0 |b 2 |
| 700 | 1 | _ | |a López, Xavier |0 P:(DE-HGF)0 |b 3 |
| 700 | 1 | _ | |a Bäumer, Christoph |0 P:(DE-Juel1)159254 |b 4 |
| 700 | 1 | _ | |a Kentzinger, Emmanuel |0 P:(DE-Juel1)130754 |b 5 |
| 700 | 1 | _ | |a Pyckhout-Hintzen, Wim |0 P:(DE-Juel1)130902 |b 6 |
| 700 | 1 | _ | |a Monakhov, Kirill |0 P:(DE-Juel1)167441 |b 7 |e Corresponding author |u fzj |
| 773 | _ | _ | |a 10.1021/acs.jpcc.7b02138 |g Vol. 121, no. 19, p. 10419 - 10429 |0 PERI:(DE-600)2256522-X |n 19 |p 10419 - 10429 |t The @journal of physical chemistry |v 121 |y 2017 |x 1932-7455 |
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