Utilization of Robust Zr-Based Metal-Organic Framework for Efficient N₂/H₂ Separation

The development of energy-efficient separation technologies for nitrogen (N₂)-hydrogen (H₂) mixtures under conventional industrial conditions remains a critical challenge. Adsorptive separation emerges as a promising strategy, contingent upon the design of high-performance adsorbents with tailored physicochemical properties. In this study, three isoreticular zirconium-based metal-organic frameworks (UiO-66, UiO-66-CH=CH₂, and UiO-66-F₄) are systematically evaluated for the purification of industrial N₂-H₂ mixed gases. By integrating static adsorption isotherms, dynamic breakthrough experiments, and molecular dynamics (MD) simulations, we comprehensively characterize the adsorption mechanisms and diffusion kinetics. The results demonstrate that UiO-66-F₄ exhibits optimal performance in capturing N₂ from N₂-H₂ mixtures under simulated industrial conditions, owing to its balanced binding affinity, high nitrogen uptake, and favorable micro-/mesoporous diffusion dynamics. This work offers a promising alternative for N₂-H₂ separation in industrial applications.