Assembling Silver Cluster-Based Organic Frameworks for Higher-Performance Hypergolic Properties

[Image: see text] Increasing research efforts have been focused on developing next-generation propellants. In this work, we demonstrated that assembling zero-dimensional (0D) silver clusters with energetic ligands into 3D metal organic frameworks (MOFs) not only inherited the short ignition delay (ID) time of the alkynyl-silver cluster but also significantly increased the output energy. Among them, the open cationic framework of ZZU-363 incorporating counter NO(3)(–) ions achieved a considerably reduced energy barrier and eventually the shortest ID time (26 ms), together with the highest volumetric energy density (40.4 kJ cm(–3)) and specific impulse (263.1 s), which is far superior to traditional hydrazine-based propellants. The underlying mechanisms are clearly revealed by theoretical calculations. This work opens a venue to significantly enhancing the hypergolic activity of metal clusters and MOFs.