First Principles Insights Into Emerging Perovskite Hydrides for Hydrogen Storage Applications: A Review

The global transition toward carbon‐neutral energy systems has intensified research on safe, efficient, and high‐density hydrogen storage materials. Among solid‐state systems, hydride perovskites have recently emerged as promising candidates due to their tunable crystal chemistry, structural versatility, and potential for reversible hydrogen absorption. However, experimental progress on hydride perovskites remains limited, and much of the current understanding is driven by first‐principles density functional theory (DFT) investigations. This review provides a comprehensive assessment of DFT studies on hydride perovskites, highlighting their structural stability, electronic behavior, mechanical properties, thermodynamic properties, and hydrogen storage performance. Moreover, practical applicability and synthesizability of DFT‐predicted hydride perovskites can be evaluated through several key computational indicators, which are discussed in detail. We critically examine the predictive capabilities of DFT in modeling these materials, discuss trends across different compositional families, and identify key descriptors that influence hydrogen uptake and release. Furthermore, we outline experimentally relevant insights derived from first‐principles calculations and propose directions for future synthesis and characterization. By consolidating theoretical advances and mapping existing knowledge gaps, this review aims to guide both computational and experimental efforts toward the practical development of perovskite‐based hydrogen storage materials.