Picturing the Gap Between the Performance and US‐DOE's Hydrogen Storage Target: A Data‐Driven Model for MgH2 Dehydrogenation

Abstract Developing solid‐state hydrogen storage materials is as pressing as ever, which requires a comprehensive understanding of the dehydrogenation chemistry of a solid‐state hydride. Transition state search and kinetics calculations are essential to understanding and designing high‐performance solid‐state hydrogen storage materials by filling in the knowledge gap that current experimental techniques cannot measure. However, the ab initio analysis of these processes is computationally expensive and time‐consuming. Searching for descriptors to accurately predict the energy barrier is urgently needed, to accelerate the prediction of hydrogen storage material properties and identify the opportunities and challenges in this field. Herein, we develop a data‐driven model to describe and predict the dehydrogenation barriers of a typical solid‐state hydrogen storage material, magnesium hydride (MgH 2 ), based on the combination of the crystal Hamilton population orbital of Mg−H bond and the distance between atomic hydrogen. By deriving the distance energy ratio, this model elucidates the key chemistry of the reaction kinetics. All the parameters in this model can be directly calculated with significantly less computational cost than conventional transition state search, so that the dehydrogenation performance of hydrogen storage materials can be predicted efficiently. Finally, we found that this model leads to excellent agreement with typical experimental measurements reported to date and provides clear design guidelines on how to propel the performance of MgH 2 closer to the target set by the United States Department of Energy (US‐DOE).