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.