RT Journal Article SR Electronic T1 Hypergolic zeolitic imidazolate frameworks (ZIFs) as next-generation solid fuels: Unlocking the latent energetic behavior of ZIFs JF Science Advances JO Sci Adv FD American Association for the Advancement of Science SP eaav9044 DO 10.1126/sciadv.aav9044 VO 5 IS 4 A1 Titi, H. M. A1 Marrett, J. M. A1 Dayaker, G. A1 Arhangelskis, M. A1 Mottillo, C. A1 Morris, A. J. A1 Rachiero, G. P. A1 Friščić, T. A1 Rogers, R. D. YR 2019 UL http://advances.sciencemag.org/content/5/4/eaav9044.abstract AB Hypergolic materials, capable of spontaneous ignition upon contact with an external oxidizer, are of critical importance as fuels and propellants in aerospace applications (e.g., rockets and spacecraft). Currently used hypergolic fuels are highly energetic, toxic, and carcinogenic hydrazine derivatives, inspiring the search for cleaner and safer hypergols. Here, we demonstrate the first strategy to design hypergolic behavior within a metal-organic framework (MOF) platform, by using simple “trigger” functionalities to unlock the latent and generally not recognized energetic properties of zeolitic imidazolate frameworks, a popular class of MOFs. The herein presented six hypergolic MOFs, based on zinc, cobalt, and cadmium, illustrate a uniquely modular platform to develop hypergols free of highly energetic or carcinogenic components, in which varying the metal and linker components enables the modulation of ignition and combustion properties, resulting in excellent hypergolic response evident by ultrashort ignition delays as low as 2 ms.