Metal hydrides are potential candidates for applications in hydrogen-related technologies, such as energy storage, hydrogen compression, and hydrogen sensing, to name just a few. However, understanding the electronic structure and chemical environment of hydrogen within them remains a key challenge. This work presents a new analytical pathway to explore these aspects in technologically relevant systems using hard x-ray photoelectron spectroscopy (HAXPES) on thin films of two prototypical metal dihydrides: YH2−δ and TiH2−δ. By taking advantage of the tunability of synchrotron radiation, a nondestructive depth profile of the chemical states is obtained using core-level spectra. Combining experimental valence-band (VB) spectra collected at varying photon energies with theoretical insights from density functional theory (DFT) calculations, a description of the bonding nature and the role of d versus sp contributions to states near the Fermi energy are provided. Moreover, a reliable determination of the enthalpy of formation is proposed by using experimental values of the energy position of metal s-band features close to the Fermi energy in the HAXPES VB spectra.
Kalha, C., Ratcliff, L.E., Colombi, G., Schlueter, C., Dam, B., Gloskovskii, A., et al. (2024). Revealing the Bonding Nature and Electronic Structure of Early-Transition-Metal Dihydrides. PRX ENERGY, 3, 013003 [10.1103/PRXEnergy.3.013003].
Revealing the Bonding Nature and Electronic Structure of Early-Transition-Metal Dihydrides
Francesco Offi;
2024-01-01
Abstract
Metal hydrides are potential candidates for applications in hydrogen-related technologies, such as energy storage, hydrogen compression, and hydrogen sensing, to name just a few. However, understanding the electronic structure and chemical environment of hydrogen within them remains a key challenge. This work presents a new analytical pathway to explore these aspects in technologically relevant systems using hard x-ray photoelectron spectroscopy (HAXPES) on thin films of two prototypical metal dihydrides: YH2−δ and TiH2−δ. By taking advantage of the tunability of synchrotron radiation, a nondestructive depth profile of the chemical states is obtained using core-level spectra. Combining experimental valence-band (VB) spectra collected at varying photon energies with theoretical insights from density functional theory (DFT) calculations, a description of the bonding nature and the role of d versus sp contributions to states near the Fermi energy are provided. Moreover, a reliable determination of the enthalpy of formation is proposed by using experimental values of the energy position of metal s-band features close to the Fermi energy in the HAXPES VB spectra.I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.
