Green synthesis of MOF-based hybrid nanostructures for efficient hydrogen storage and regeneration

Hydrogen (H?) is an important clean energy carrier to offset fossil fuel dependence, but its storage and regeneration present considerable barriers to mass penetration. Metal-organic frameworks (MOFs), marked by high porosity (>3000 m²/g) and structural flexibility, represent an extremely promising class of materials for reversible physisorption and chemisorption of H?. This review critically evaluates green synthesis methods—mechanochemical, sonochemical, and plasma-assisted synthesis—and their reduced solvents and energy inputs, which facilitate scale-up synthesis of MOFs and hybrids thereof with conjugated polymers (polythiophenes), small molecules (benzothiophene derivatives), and nanomaterials (graphene). These methods provide structures with enhanced binding enthalpies, mechanical stability, and regeneration potential, with >5 wt% uptake at near-ambient conditions (298 K, 100 bar) and >1500 cycles. Significant advances in functionalized linkers (e.g., amino- or halogen-substituted BDC) and bimetallic MOFs are showcased, including computational modeling (Grand Canonical Monte Carlo, DFT) and high-end characterization (synchrotron SAXS/WAXS, nanoindentation). Instability upon cycling and scale-up with economic factors are also considered, with an emphasis on integrating photocatalytic functionalities for in-situ H? generation from water. Directions of the future encompass multifunctional systems for vehicular and urban energy applications that align with DOE goals and sustainable development needs. This exhaustive analysis provides a roadmap to realize MOF-based breakthroughs as practical clean energy applications.

Dr. Laya Anjo is a Scientist at the Advanced Materials and Microdevices Laboratory, CANDLE Synchrotron Research Institute, Yerevan, Armenia. She holds expertise in nanotechnology and advanced materials with a focus on Metal–Organic Frameworks (MOFs) for clean energy applications, including hydrogen storage and carbon capture. Her current research involves the development of high-temperature synthesis techniques for submicron powders and thin films, as well as the design of novel nanostructured systems for energy and environmental technologies. She has authored and co-authored several scientific papers and actively participates in international collaborations and conferences.