Abstract
Magnesium dihydride (MgH2) stores 7.7 wt % hydrogen but it suffers from a high thermodynamic stability and slow (de)hydrogenation kinetics. Alloying Mg with lightweight transition metals (TM) (=Sc,Ti,V,Cr) aims at improving the thermodynamic and kinetic properties. We study the structure and stability of MgxTM1−xH2 compounds, x=[0–1], by first-principles calculations at the level of density functional theory. We find that the experimentally observed sharp decrease in hydrogenation rates for x0.8 correlates with a phase transition of MgxTM1−xH2 from a fluorite to a rutile phase. The stability of these compounds decreases along the series Sc, Ti, V, and Cr. Varying the TM and the composition x, the formation enthalpy of MgxTM1−xH2 can be tuned over the substantial range of 0–2 eV/f.u. Assuming however that the alloy MgxTM1−x does not decompose upon dehydrogenation, the enthalpy associated with reversible hydrogenation of compounds with a high magnesium content (x=0.75) is close to that of pure Mg.
Original language | Undefined |
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Pages (from-to) | 024105/1-024105/8 |
Number of pages | 8 |
Journal | Physical review B: Condensed matter and materials physics |
Volume | 79 |
Issue number | 2 |
DOIs | |
Publication status | Published - 2009 |
Keywords
- enthalpy
- vanadium compounds
- titanium compounds
- density functional theory
- magnesium compounds
- heat of formation
- IR-68604
- hydrogen storage
- scandium compounds
- Chromium compounds
- Ab initio calculations
- METIS-257190
- solid-state phase transformations