Stabilizing $\gamma$-MgH${}_2$ at Nanotwins in Mechanically Constrained Nanoparticles

Abstract

Reversible hydrogen uptake and the metal/dielectric transition make the Mg/MgH${}_2$ system a prime candidate for solid state hydrogen storage and dynamic plasmonics. However, high dehydrogenation temperatures and slow dehydrogenation hamper broad applicability. One promising strategy to improve dehydrogenation is the formation of metastable $\gamma$-MgH${}_2$. A nanoparticle (NP) design, where $\gamma$-MgH${}_2$ forms intrinsically during hydrogenation is presented and a formation mechanism based on transmission electron microscopy results is proposed.Volume expansion during hydrogenation causes compressive stress within the confined, anisotropic NPs, leading to plastic deformation of $\beta$-MgH${}_2$ via (301) $\beta$ twinning. It is proposed that these twins nucleate $\gamma$-MgH${}_2$ nanolamellas, which are stabilized by residual compressive stress. Understanding this mechanism is a crucial step toward cycle-stable, Mg-based dynamic plasmonic and hydrogen-storage materials with improved dehydrogenation. It is envisioned that a more general design of confined NPs utilizes the inherent volume expansion to reform $\gamma$-MgH${}_2$ during each rehydrogenation

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Cited by in corpus (1)

• Stabilizing $\gamma$-MgH${}_2$ at Nanotwins in Mechanically Constrained Nanoparticles