Pure-silica zeolites: advances in synthesis, atomic-scale structural determination, and applications.

Pure-silica zeolites have become indispensable in adsorption, separation, and catalysis under demanding conditions, owing to their exceptional structural diversity, hydrophobicity, thermal and chemical stability, and tunable pore architectures. A comprehensive understanding-spanning synthesis, atomic-scale structural determination, and application-is essential for advancing sustainable chemical processes, green catalysis, and next-generation separation technologies. Our review systematically evaluates the structural features of two-dimensional (2D) layered and three-dimensional (3D) framework zeolites, comparatively assesses the advantages, limitations, and applicability of various synthesis strategies, and critically examines the fundamental principles, strengths, inherent limitations, and recent advances in state-of-the-art structural characterization techniques. We further summarize their major applications in adsorption, separation, and catalysis. By uniquely integrating synthesis, structure, and function, our review provides an up-to-date resource that reflects current challenges, emerging opportunities, and promising directions for further research in pure-silica zeolites.