Stereochemical Control of Static Strength and Dynamic Fracture for Efficient Atomization of Supramolecular Gel Propellants

Supramolecular gel propellants immobilize liquid fuels through the efficient self-assembly of low-molecular-weight gelators, enabling storage-stable networks at minimal additive loading while remaining susceptible to rapid disruption during atomization. However, the multiscale relationships linking molecular design, supramolecular organization, rheology, and atomization remain poorly understood. Here, four glutamic acid-derived low-molecular-weight gelators were developed by varying molecular chirality, steric hindrance around hydrogen-bonding sites, and alkyl-chain length to regulate their assembly in aviation fuel JP-10. Comparison of racemic and enantiopure analogues highlighted stereochemical coherence as a key determinant of higher-order non-covalent assembly. G4, bearing an N-acetyl headgroup, an enantiopure L-glutamic acid configuration, and C18 alkyl chains, exhibited the highest gelation efficiency and formed ordered lamellar packing and an interconnected helical nanofiber network. The resulting G4@JP-10 gel combined a high yield stress of 718.50 Pa with a low critical strain of approximately 40%, resisting the onset of flow under weak perturbations while showing limited tolerance to large deformation under strong external shear. The test results of low-field nuclear magnetic resonance (LF-NMR) indicated weak network-imposed restriction of JP-10 molecular motion, while the shear-disrupted G4 sample exhibited the lowest average surface tension of 28.34 mN m-1, reducing capillary resistance to new gas–fuel interface formation. Consequently, G4 achieved a Sauter mean diameter (SMD) of 5.38 μm at a N2 pressure of 0.6 MPa, lower than that of neat JP-10 under identical conditions. This work reveals the unique advantages of chiral supramolecular gels for propellant atomization and establishes comprehensive structure–property relationships that bridge molecular structure and assembly behavior with rheological characteristics and atomization performance.