Beyond batteries: Architecting materials through surface chemistry and engineering for revolutionizing hydrogen storage

As the world races toward decarbonization, hydrogen has emerged as the hub of sustainable energy storage, boasting an energy density triple that of gasoline and zero-emission potential. Yet its widespread adoption faces triads critical roadblock, namely, no existing storage solution simultaneously achieves high capacity, ambient operation, and economic viability. This review shatters conventional paradigms by revealing how atomic-scale surface chemistry and engineering can unlock full potential of hydrogen. The review presents a groundbreaking perspective that surpasses traditional storage classifications, demonstrating how MXenes functionalized with quantum dots can enhance H₂ spillover at room temperature, while Artificial intelligence (AI)- and machine learning-designed metal-organic frameworks (MOFs) achieve record uptake at near-ambient conditions. Also, it unveils a new class of dynamic metal hydrides that defy pressure-dependent limitations and 2D boron nitride membranes enabling selective hydrogen sieving, breakthroughs that render conventional compressed gas and cryogenic approaches obsolete. Crucially, the review exposes the hidden potential of defect engineering, showing how strategically placed vacancies in nanoconfined hydrides can lower dehydrogenation barriers by 100 °C. The analysis of hybrid architectures from MOF-MXene composites to catalytic liquid organic hydrogen carriers (LOHCs) provides the first unified framework for overcoming the reversibility-stability trade-off that has plagued the field for decades. For these reasons, by bridging fundamental surface chemistry and engineering to hybrid material design and AI-driven optimization, this review not only synthesizes the latest research but also charts a clear path toward practical, high-performance hydrogen storage solutions. Accordingly, this work delivers an actionable roadmap for materials that do not just store hydrogen, but actively engineer its behaviour. Hence, the insights contained herein could accelerate the hydrogen economy by decades, transforming what was once chemistry's hardest problem into our most powerful solution for a fossil fuel-free future.