Hydrogen Energy Storage via Carbon-Based Materials: From Traditional Sorbents to Emerging Architecture Engineering and AI-Driven Optimization

Hydrogen is widely recognized as a key enabler of the clean energy transition, but the lack of safe, efficient, and scalable storage technologies continues to hinder its broad deployment. Conventional hydrogen storage approaches, such as compressed hydrogen storage, cryo-compressed hydrogen storage, and liquid hydrogen storage, face limitations, including high energy consumption, elevated cost, weight, and safety concerns. In contrast, solid-state hydrogen storage using carbon-based adsorbents has gained growing attention due to their chemical tunability, low cost, and potential for modular integration into energy systems. This review provides a comprehensive evaluation of hydrogen storage using carbon-based materials, covering fundamental adsorption mechanisms, classical materials, emerging architectures, and recent advances in computationally AI-guided material design. We first discuss the physicochemical principles driving hydrogen physisorption, chemisorption, Kubas interaction, and spillover effects on carbon surfaces. Classical adsorbents, such as activated carbon, carbon nanotubes, graphene, carbon dots, and biochar, are evaluated in terms of pore structure, dopant effects, and uptake capacity. The review then highlights recent progress in advanced carbon architectures, such as MXenes, three-dimensional architectures, and 3D-printed carbon platforms, with emphasis on their gravimetric and volumetric performance under practical conditions. Importantly, this review introduces a forward-looking perspective on the application of artificial intelligence and machine learning tools for data-driven sorbent design. These methods enable high-throughput screening of materials, prediction of performance metrics, and identification of structure–property relationships. By combining experimental insights with computational advances, carbon-based hydrogen storage platforms are expected to play a pivotal role in the next generation of energy storage systems. The paper concludes with a discussion on remaining challenges, utilization scenarios, and the need for interdisciplinary efforts to realize practical applications.