Morphology-engineered MOFs for advanced carbon capture and separation: From zero-dimensional particles to three-dimensional architectures

Metal-organic frameworks (MOFs) have emerged as forefront materials for carbon capture and separation due to their structural tunability and ultrahigh porosity. However, their inherent powder morphology poses significant challenges for industrial implementation, including handling difficulties, pressure drop issues, and device integration limitations. This review systematically examines the burgeoning field of morphology engineering as a critical strategy to bridge this lab-to-industry gap. The design principles and synthesis methodologies for tailoring MOFs across dimensional scales were primarily delineated, including modulated synthesis, in-situ growth and post-synthetic treatment. Then a comprehensive analysis is provided for zero-dimensional granules/pellets and core-shell structures designed for fixed-bed adsorbers, two-dimensional membranes and thin films optimized for energy-efficient separation, and three-dimensional monoliths, aerogels, and foams that integrate hierarchical porosity for enhanced mass transport and mechanical integrity. For each dimensional class, we discuss the governing mechanisms (e.g., molecular sieving, selective surface diffusion, competitive adsorption), evaluate key performance metrics (uptake capacity, selectivity, kinetics), and critically assess industrial suitability in terms of scalability, mechanical stability, and process compatibility. Finally, we highlight future frontiers, emphasizing the need for advanced shaping techniques like 3D printing, the rational design of multi-scale architectures, and the co-optimization of material properties with system engineering to realize the full potential of MOFs in practical carbon management technologies. This review aims to serve as a roadmap for developing high-performance, application-specific MOF morphologies to accelerate the deployment of next-generation carbon capture systems.