A novel ADN/TANPDO supramolecular crystal with anti-hygroscopicity and high energy: A promising strategy to construct advanced propellant materials

•Utilizing molecular self-assembly method effectively reduces the hygroscopicity without compromising energetic performance of ADN (ammonium dinitramide).•A novel ADN/TANPDO (2,4,6-triamino-5-nitropyrimidine-1,3-dioxide) supramolecular crystal was obtained through a rapid, green, efficient, and scalable self-assembly method.•The ADN/TANPDO supramolecular crystals exhibit good comprehensive performances, making its potential as a new propellant material.•This study offers an effective strategy for solving the strong hygroscopicity of materials and presents a novel method for developing advanced propellant materials in the future. Herein, encapsulating NH4+ ions through molecular self-assembly method has been employed to reduce the strong hygroscopicity of ADN (ammonium dinitramide). A novel ADN/TANPDO (2,4,6-triamino-5-nitropyrimidine-1,3-dioxide) supramolecular crystal with a 3:2 ratio was obtained using a rapid, green, efficient, and scalable self-assembly method. Compared with pure ADN, ADN/TANPDO supramolecular crystal exhibits a significantly lower hygroscopicity rate of 2.76 % (25 °C and 75 % relative humidity) and a lower impact sensitivity of 15 J, as well as a markedly higher specific impulse of 236 s. Additionally, the propellant formulation based on ADN/TANPDO supramolecular crystal presents high predicted energy with decreased content of HCl gas, making it a promising candidate for a high-energy and low-characteristic signal propellant component. Furthermore, this work offers a promising strategy to construct supramolecular crystals for solving the strong hygroscopicity of ADN and simultaneously assemble oxidizers with high-energy materials together at the molecular scale to achieve advanced propellant materials in the future.