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Varying the Alkali-Metal Radii in (KxRb1−x)n[GaH2]n (0 ≤ x ≤ 1)Reorients a Stable Polyethylene-Structured [GaH2]nn− Anionic Chain
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
2013 (English)In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 52, no 9, 4771-4773 p.Article in journal (Refereed) Published
Abstract [en]

The stability of a negatively chargedpolyethylene-structured [GaH2]nn−cluster ion was inves-tigated by varying the K+/Rb+ratio in (KxRb1−x)n[GaH2]n(0≤x≤1). Neutron, X-ray, and IR spectroscopies wereused to characterize the new phases. Between the limitingcompositions Kn[GaH2]nand Rbn[GaH2]n, the [GaH2]nn−chains remained almost identical, indicating a stable specie.For rubidium-rich samples up to a potassium contentcorresponding to (K0.5Rb0.5)n[GaH2]n, two phases coexistin the samples, RbGaH2and (K0.5Rb0.5)n[GaH2]n, with aratio mirroring the relative alkali-ion content. The twophases have a different alignment of the [GaH2]nn−chains.For potassium-rich samples beyond (K0.5Rb0.5)n[GaH2]n,the samples were single-phased. The unit cell volume ofthe new (K0.5Rb0.5)n[GaH2]nstructure type shrinksaccording to Vegard’s law as smaller K+ions substitutefor larger Rb+ions. The [GaH2]nn−chains remained,however, almost identical. IR spectra from the differentphases were very similar, exhibited stretching, scissoring,and rocking modes similar to those in ordinary poly-ethylene, but shifted to lower frequencies, reflectingweaker Ga−H bonds. The existence of stable Kn[GaH2]nand Rbn[GaH2]n, would help to dehydrogenate KGaH4and RbGaH4upon heating. If this could be transferred tolighter alanates and borohydrides, it could be possible todevelop more functional hydrogen-storage systems.

Place, publisher, year, edition, pages
2013. Vol. 52, no 9, 4771-4773 p.
National Category
Inorganic Chemistry
Research subject
Structural Chemistry
Identifiers
URN: urn:nbn:se:su:diva-89752DOI: 10.1021/ic400224aISI: 000318669400009OAI: oai:DiVA.org:su-89752DiVA: diva2:619918
Funder
Swedish Energy Agency
Note

AuthorCount: 3;

Available from: 2013-05-07 Created: 2013-05-07 Last updated: 2017-12-06Bibliographically approved
In thesis
1. Transition Metal Hydride Complexes and Hydrogenated Gallium Clusters: Synthesis and Structural Properties
Open this publication in new window or tab >>Transition Metal Hydride Complexes and Hydrogenated Gallium Clusters: Synthesis and Structural Properties
2013 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Synthesis and structural characterisation of metal hydrides in two important systems are presented. The first system presented is low valent cobalt and nickel complex hydrides with the compositions BaMg5Co2H10, RbMg5CoNiH10, SrMg2CoH7and Sr4Mg4Co3H19 featuring nickel with oxidation state of 0 and cobalt with oxidation state +I and -I. The second system presented is polyanionic gallium complex hydrides with the compositions RbGaH2, RbxK(1−x)GaH2 (0.5≤x≤1), CsxRb(8−x)Ga5H15 (0≤x≤8) and Cs10Ga9H25 featuring novel hydrogenous polyanionic gallium hydride clusters mimicking common hydrocarbons. The syntheses of the compounds were performed at elevated temperatures and at moderate hydrogen pressures (50-100 bar). The structural investigations were mainly done by X-ray powder diffraction (XRPD) and neutron powder diffraction (NPD). The metal-hydrogen bond was investigated by vibrational spectroscopy using Fourier Transform IR-spectroscopy (FTIR) and Inelastic Neutron Scattering (INS).By subtle changes in the compositions of the hydrides it was possible to induce major changes in band gaps, oxidation states and structures.

Place, publisher, year, edition, pages
Stockholm: Department of Materials and Environmental Chemistry (MMK), Stockholm University, 2013. 64 p.
Keyword
Metal hydrides, Solid state Synthesis, X-ray diffraction, Neutron Scattering
National Category
Inorganic Chemistry
Research subject
Structural Chemistry
Identifiers
urn:nbn:se:su:diva-89760 (URN)978-91-7447-711-5 (ISBN)
Public defence
2013-06-05, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

At the time for the doctoral defence the following papers were unpublished and had a status as follows: Paper 1: Manuscript; Paper 2: Accepted; Paper 5: Manuscript

Available from: 2013-05-14 Created: 2013-05-07 Last updated: 2013-05-07Bibliographically approved

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