Enhanced Structural Decoupling and Spatiotemporal Evolution of Thermal–Mass Coupling in LaNi5-Based Solid-State Hydrogen Storage Reactors

Hydrogen energy is pivotal to the global energy transition, and the development of high-efficiency, safe hydrogen storage technologies constitutes a prerequisite for its large-scale commercialization. Kinetic bottlenecks including slow reactions, delayed front propagation, and marked spatial heterogeneity driven by strong thermal–mass transfer coupling restrict the engineering application of solid-state metal hydrides. However, the current research mainly focusing on overall performance lacks a systematic understanding of the spatiotemporal evolution mechanisms and their intrinsic links to internal structural control. In this work, a 3D multiphysics model of a LaNi5-based reactor is developed to systematically elucidate spatiotemporal evolution patterns, facilitating the proposal of a structural decoupling framework based on synergistic thermal–mass resistance reconfiguration. Both absorption and desorption show distinct three-stage evolution, shifting from kinetic dominance to transfer limitation: absorption causes core self-inhibition via heat-hydrogen supply mismatch, leading to much lower core than surface storage capacity; desorption results in significant inner-layer lag due to endothermic cooling-driven pressure drops. Thermal–mass coupling-induced inverted spatiotemporal evolution is identified as the root cause of spatial heterogeneity. Quantitative comparison of straight-pipe, spiral-tube, and honeycomb structures reveals that internal architectures achieve effective thermal–mass decoupling through expanded heat-exchange areas, reconstructed diffusion pathways, and optimized heat source distribution. Notably, the honeycomb structure with a parallel micro-unit network achieves 89.1% and 86.6% reductions in absorption and desorption times, respectively, showing superior dynamic performance and field uniformity. This study provides a theoretical basis for the mechanism-driven design and synergistic performance optimization of high-efficiency solid-state hydrogen storage reactors.