Evidence of Intermediate Hydrogen States in the Formation of a Complex Hydride
Abstract
A complex hydride (LaMg2NiH7) composed of La3+, two Mg2+, [NiH4]4– with a covalently bonded hydrogen, and three H– was formed from an intermetallic LaMg2Ni via an intermediate phase (LaMg2NiH4.6) composed of La, Mg, NiH2, NiH3 units, and H atoms at tetrahedral sites. The NiH2 and NiH3 units in LaMg2NiH4.6 were reported as precursors for [NiH4]4– in LaMg2NiH7 [Miwa et al. J. Phys. Chem. C 2016, 120, 5926–5931]. To further understand the hydrogen states in the precursors (the NiH2 and NiH3 units) and H atoms at the tetrahedral sites in the intermediate phase, LaMg2NiH4.6, we observed the hydrogen vibrations in LaMg2NiH4.6 and LaMg2NiH7 by using inelastic neutron scattering. A comparison of the hydrogen vibrations of the NiH2 and NiH3 units with that of [NiH4]4– shows that the librational modes of the NiH2 and NiH3 units were nonexistent; librational modes are characteristic modes for complex anions, such as [NiH4]4–. Furthermore, the hydrogen vibrations for the H atoms in the tetrahedral sites showed a narrower wavenumber range than that for H– and a wider range than that for typical interstitial hydrogen. The results indicated the presence of intermediate hydrogen states before the formation of [NiH4]4– and H–.
- Authors:
-
- Tohoku Univ., Sendai (Japan). Inst. for Materials Research
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division, Neutron Sciences Directorate
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division, Neutron Sciences Directorate
- Tohoku Univ., Sendai (Japan). Inst. for Materials Research; Tohoku Univ., Sendai (Japan). WPI-Advanced Inst. for Materials Research
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program; Japan Society for the Promotion of Science (JSPS)
- OSTI Identifier:
- 1422532
- Grant/Contract Number:
- AC05-00OR22725; 16K06766; 25220911
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Inorganic Chemistry
- Additional Journal Information:
- Journal Volume: 57; Journal Issue: 2; Journal ID: ISSN 0020-1669
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Inelastic neutron scattering; complex hydride; hydrogen state
Citation Formats
Sato, Toyoto, Ramirez-Cuesta, Anibal J., Daemen, Luke L., Cheng, Yongqiang, and Orimo, Shin-ichi. Evidence of Intermediate Hydrogen States in the Formation of a Complex Hydride. United States: N. p., 2017.
Web. doi:10.1021/acs.inorgchem.7b02834.
Sato, Toyoto, Ramirez-Cuesta, Anibal J., Daemen, Luke L., Cheng, Yongqiang, & Orimo, Shin-ichi. Evidence of Intermediate Hydrogen States in the Formation of a Complex Hydride. United States. https://doi.org/10.1021/acs.inorgchem.7b02834
Sato, Toyoto, Ramirez-Cuesta, Anibal J., Daemen, Luke L., Cheng, Yongqiang, and Orimo, Shin-ichi. Tue .
"Evidence of Intermediate Hydrogen States in the Formation of a Complex Hydride". United States. https://doi.org/10.1021/acs.inorgchem.7b02834. https://www.osti.gov/servlets/purl/1422532.
@article{osti_1422532,
title = {Evidence of Intermediate Hydrogen States in the Formation of a Complex Hydride},
author = {Sato, Toyoto and Ramirez-Cuesta, Anibal J. and Daemen, Luke L. and Cheng, Yongqiang and Orimo, Shin-ichi},
abstractNote = {A complex hydride (LaMg2NiH7) composed of La3+, two Mg2+, [NiH4]4– with a covalently bonded hydrogen, and three H– was formed from an intermetallic LaMg2Ni via an intermediate phase (LaMg2NiH4.6) composed of La, Mg, NiH2, NiH3 units, and H atoms at tetrahedral sites. The NiH2 and NiH3 units in LaMg2NiH4.6 were reported as precursors for [NiH4]4– in LaMg2NiH7 [Miwa et al. J. Phys. Chem. C 2016, 120, 5926–5931]. To further understand the hydrogen states in the precursors (the NiH2 and NiH3 units) and H atoms at the tetrahedral sites in the intermediate phase, LaMg2NiH4.6, we observed the hydrogen vibrations in LaMg2NiH4.6 and LaMg2NiH7 by using inelastic neutron scattering. A comparison of the hydrogen vibrations of the NiH2 and NiH3 units with that of [NiH4]4– shows that the librational modes of the NiH2 and NiH3 units were nonexistent; librational modes are characteristic modes for complex anions, such as [NiH4]4–. Furthermore, the hydrogen vibrations for the H atoms in the tetrahedral sites showed a narrower wavenumber range than that for H– and a wider range than that for typical interstitial hydrogen. The results indicated the presence of intermediate hydrogen states before the formation of [NiH4]4– and H–.},
doi = {10.1021/acs.inorgchem.7b02834},
journal = {Inorganic Chemistry},
number = 2,
volume = 57,
place = {United States},
year = {2017},
month = {12}
}
Web of Science
Figures / Tables:

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