Extracting an Empirical Intermetallic Hydride Design Principle from Limited Data via Interpretable Machine Learning

An open question in the metal hydride community is whether there are simple, physics-based design rules that dictate the thermodynamic properties of these materials across the variety of structures and chemistry they can exhibit. While black box machine learning-based algorithms can predict these properties with some success, they do not directly provide the basis on which these predictions are made, therefore complicating the a priori design of novel materials exhibiting a desired property value. In this work we demonstrate how feature importance, as identified by a gradient boosting tree regressor, uncovers the strong dependence of the metal hydride equilibrium H₂ pressure on a volume-based descriptor that can be computed from just the elemental composition of the intermetallic alloy. Elucidation of this simple structure–property relationship is valid across a range of compositions, metal substitutions, and structural classes exhibited by intermetallic hydrides. Finally, this permits rational targeting of novel intermetallics for high-pressure hydrogen storage (low-stability hydrides) by their descriptor values, and we predict a known intermetallic to form a low-stability hydride (as confirmed by density functional theory calculations) that has not yet been experimentally investigated.