Advances in single-crystal framework materials: Design, synthesis, and applications

Porous materials are integral to numerous aspects of daily life, from metabolic processes in the human body to various industrial applications. Significant efforts have been directed toward the synthesis of single-crystalline reticular materials with well-defined architectures and enhanced performance by reticulating organic units into extended frameworks. However, the development of these materials for diverse applications is substantially impeded by the limitations of current preparation strategies and the unclear mechanisms underlying single-crystal formation. This review provides a comprehensive summary of recent advancements in the design and synthetic methodologies of single-crystal framework materials, emphasizing solvothermal-induced direct synthesis, template-assisted synthesis, and modulator-assisted preparation. Detailed insights into the challenges of modulating crystal growth are presented. Furthermore, the review discusses the potential large-scale applications of single-crystal frameworks, including catalysis, adsorption/separation, sensing, polarized optics, and life sciences, thereby broadening the scope of their utility across various fields. • Synthesis methods for single-crystal framework materials (SCFM) • Applications of SCFM in catalysis, adsorption, sensing, polarized optics, and life sciences • Detailed insights into the challenges of modulating crystal growth • Outlook of SCFM from the synthesis, the structure identification to the relationship of structure-performance