Cyano‐Bridged Metal Frameworks as Emerging Catalysts for Small Molecule Conversion

Cost‐effective catalysts are pivotal in addressing energy and environmental challenges through the catalytic conversion of small molecules. Cyano‐bridged metal frameworks (CMFs), as a subclass of reticular materials, demonstrate potential in small molecule conversion. However, CMFs are conventionally utilized as precursors for derivative synthesis, which inadvertently overshadows their intrinsic properties. Recent research has revealed that CMFs have emerged as direct catalysts. Accordingly, the feasibility is investigated of directly employing CMFs as catalysts for small molecule conversion and propose integrated design strategies encompassing element selection, structural modulation, and adaptation to working conditions. Specifically, insights is offered into the rational selection and combination of building units based on an updated understanding of CMFs' coordination environments. A crystallization‐kinetics‐guided, multi‐dimensional assembly methodology is further proposed to achieve structural diversity and topological complexity. Finally, the application potential is demonstrated of CMFs in small molecule conversion through experimental evaluation and theoretical analysis of key intrinsic material properties. This study establishes a conceptual and methodological foundation for advancing CMFs toward broader applications in small molecule conversion.