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Chemically Stable Group IV-V Transition Metal Carbide Thin Films in Hydrogen Radical Environments

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arXiv:2404.14108v1 Announce Type: cross
Abstract: Hydrogen is playing a crucial role in the green energy transition. Yet, its tendency to react with and diffuse into surrounding materials poses a challenge. Therefore, it is critical to develop coatings that protect hydrogen-sensitive system components in reactive-hydrogen environments. In this work, we report group IV-V transition metal carbide (TMC) thin films as potential candidates for hydrogen-protective coatings in hydrogen radical (H*) environments at elevated temperatures. We identify three classes of TMCs based on the reduction of carbides and surface oxides (TMOx). HfC, ZrC, TiC, TaC, NbC, and VC (class A) are found to have a stable carbidic-C (TM-C) content, with a further sub-division into partial (class A1: HfC, ZrC, and TiC) and strong (class A2: TaC, NbC, and VC) surface TMOx reduction. In contrast to class A, a strong carbide reduction is observed in Co2C (class B), along with a strong surface TMOx reduction. The H*-TMC/TMOx interaction is hypothesized to entail three processes: (i) hydrogenation of surface C/O-atoms, (ii) formation of CHx/OHx species, and (iii) subsurface C/O-atoms diffusion to the surface vacancies. The number of adsorbed H-atoms required to form CHx/OHx species (i), and the corresponding energy barriers (ii) are estimated based on the change in the Gibbs free energy (DeltaG) for the reduction reactions of TMCs and TMOx. Hydrogenation of surface carbidic-C-atoms is proposed to limit the reduction of TMCs, whereas the reduction of surface TMOx is governed by the thermodynamic barrier for forming H2O.

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