Transformation Journey of Zr‐Based Metal–Organic Frameworks: Study on Mechanics and Hydrogen Storage Under Doping Regulation

This study delves into the transformation journey of Zr-based metal-organic frameworks (MOFs), focusing on enhancing their mechanical properties and hydrogen storage capacities through doping regulation. MOFs, a versatile class of crystalline porous materials, have garnered significant attention due to their unique properties and broad potential applications in gas storage, separation, catalysis, and sensing. Among them, Zr-based MOFs stand out for their exceptional stability and high surface area. This study employs multiscale computational methods, including molecular dynamics simulations, grand canonical Monte Carlo simulations, and density functional theory, to conduct systematic research on six mainstream Zr-based MOF materials (UiO-66, UiO-67, UiO-68, MOF-801, MOF-802, and MOF-841). Under the conditions of 66 K and 1 bar, it explores the influence of metal ion substitution (Fe, Co, Ni, Cu, and Zn) on their mechanical properties and hydrogen storage performance. The study reveals that metal ion substitution can significantly regulate the structural stability and hydrogen adsorption capacity of Zr-based MOFs, providing an important basis for the design and optimization of high-performance MOF functional materials.