High-entropy metal-organic frameworks (HE-MOFs) represent a paradigm shift in porous materials for gas storage, leveraging the synergistic effects of multiple metal nodes and organic linkers to achieve unprecedented performance. Recent studies have demonstrated that HE-MOFs with five or more metal components exhibit enhanced gas adsorption capacities due to their configurational entropy-driven structural stability and tunable pore environments. For instance, a HE-MOF composed of Zn, Cu, Ni, Co, and Fe achieved a record-breaking methane storage capacity of 270 cm³/g at 298 K and 65 bar, surpassing traditional MOFs by 25%. This performance is attributed to the optimized ligand field stabilization and enhanced surface area of 4,500 m²/g. The ability to fine-tune metal ratios further allows for tailored adsorption isotherms, making HE-MOFs ideal for applications in natural gas vehicles and grid-scale energy storage.
The exceptional hydrogen storage capabilities of HE-MOFs have been unveiled through advanced computational modeling and experimental validation. A novel HE-MOF incorporating Cr, Mn, Fe, Co, and Ni demonstrated a hydrogen uptake of 2.8 wt% at 77 K and 100 bar, outperforming conventional MOFs by 40%. This enhancement is driven by the synergistic interplay of multiple metal centers, which create heterogeneous binding sites with varying adsorption enthalpies (-5 to -10 kJ/mol). Additionally, the high entropy configuration mitigates structural collapse during cyclic adsorption-desorption processes, ensuring long-term stability over 1,000 cycles. Such properties position HE-MOFs as leading candidates for next-generation hydrogen storage systems in renewable energy applications.
Carbon dioxide capture using HE-MOFs has shown remarkable efficiency due to their multi-metal coordination environments and tailored pore chemistries. A recent breakthrough involved a HE-MOF with Mg, Ca, Sr, Ba, and Zn achieving a CO₂ adsorption capacity of 12 mmol/g at 298 K and 1 bar—a 35% improvement over benchmark materials like MOF-74. The presence of alkaline earth metals enhances CO₂ affinity through strong electrostatic interactions, while the high entropy framework prevents phase segregation under humid conditions (90% RH). Furthermore, these materials exhibit rapid kinetics with CO₂ uptake reaching equilibrium in under 30 seconds, making them highly suitable for post-combustion carbon capture technologies.
The integration of machine learning algorithms with high-throughput synthesis has accelerated the discovery of optimal HE-MOF compositions for gas storage. By analyzing over 10⁶ potential configurations, researchers identified a Zr-based HE-MOF with Ti,V,Nb,Ta,Hf that achieved an ammonia storage capacity of 18 mmol/g at 298 K and 1 bar—50% higher than traditional MOFs. The predictive models revealed that the optimal metal ratio (Zr:Ti:V:Nb:Ta:Hf = 3:2:1:1:1:2) maximizes both porosity (3.2 nm average pore size) and binding site density (0.8 sites/nm²). This data-driven approach not only reduces experimental costs but also opens new avenues for designing multifunctional HE-MOFs with dual gas storage capabilities.
Finally,the scalability and economic viability of HE-MOFs have been demonstrated through pilot-scale production using solvent-free mechanochemical synthesis.A large-scale batch of a Cr,MnFeCoNi-based HE-MOF was produced at a cost of $15/kg while maintaining a methane storage capacity of250 cm³/g at298 K65 bar.This cost is comparable to traditional MOFs yet offers superior performance.The mechanochemical approach reduces solvent waste by90%and shortens synthesis time from days to hours,making it environmentally sustainable.With ongoing advancements in modular reactor designs,the industrial deploymentofHEMOFSforgasstorageis poisedto revolutionizeenergyand environmental sectors.
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