Rising Up: Hierarchical Metal-Organic Frameworks in Experiments and Simulations

Controlled synthesis across several length scales, ranging from discrete molecular building blocks to size- and morphology-controlled nanoparticles to 2D sheets and thin films and finally to 3D architectures, is an advanced and highly active research field within both the metal-organic framework (MOF) domain and the overall material science community. Along with synthetic progress, theoretical simulations of MOF structures and properties have shown tremendous progress in both accuracy and system size. Further advancements in the field of hierarchically structured MOF materials will allow the optimization of their performance; however, this optimization requires a deep understanding of the different synthesis and processing techniques and an enhanced implementation of material modeling. Such modeling approaches will allow us to select and synthesize the highest-performing structures in a targeted rational manner. Here, recent progress in the synthesis of hierarchically structured MOFs and multiscale modeling and associated simulation techniques is presented, along with a brief overview of the challenges and future perspectives associated with a simulation-based approach toward the development of advanced hierarchically structured MOF materials.