A combined experimental and theoretical study of the thermal decomposition mechanism and kinetics of ammonium dinitramide (ADN). (14th April 2020)

• Record Type: Journal Article
• Authors: Wang, Kuan; Xue, Bing; Chen, Jian-Gang; He, Zhen-Hong; Ji, Yueping; Wang, Bozhou; Lu, Jian; Liu, Zhong-Wen; Liu, Zhao-Tie
• Is Part Of: New journal of chemistry. Volume 44:Number 17(2020)
• Page Start: 6833
• Page End: 6844
• Publication Date: 2020-04-14
• Subjects: Chemistry -- Periodicals; Chimie -- Périodiques; 540
• DOI: 10.1039/c9nj06246g
• Languages: English
• ISSNs: 1144-0546

Abstract

Abstract : An overall decomposition mechanism of ammonium dinitramide was systematically investigated via DFT calculations and thermogravimetry-Fourier transform infrared-mass spectrometer (TG-FTIR-MS) techniques. Abstract : In the present study, an overall decomposition mechanism of ammonium dinitramide (ADN) in the gas phase via density functional theory (DFT) calculations was studied. Thermogravimetry-Fourier transform infrared (TG-FTIR) and thermogravimetry-mass spectrometer (TG-MS) techniques were used to verify the calculation results. In the thermal decomposition of gaseous ADN (ADN(g)), ADN(g) first decomposed into dinitraminic acid (HDN) and NH3, followed by HDN decomposition into other products with small molecules. HDN is found to isomerize into five isomers (HDN-1–5) in the gas phase. For the initial decomposition of HDN, the favorable decomposition pathway of HDN-4 (a structure of HON(O)NNO2 ) is more likely to form HNO3 and N2 O with a huge release of energy (approximately 45 kcal mol −1 ). Moreover, product HNO3 and NH3 can first combine to form NH4 NO3 . Both calculated and experimental results indicate that the product N2 O is first formed in the thermal decomposition of ADN(g). Moreover, the formation mechanism and kinetics of other products (NH3, H2 O, NO, N2 O, NO2, HONO, HNO3, etc. ) were also studied and proposed in the thermal decomposition of gaseous ADN. Overall, the systematic mechanistic investigations have provided new and detailed insights on the mechanism and kinetics of the thermal decomposition of gaseous ADN as well as informative factors to further improve the experimental performances, which can surely be beneficial to other energetic material syntheses.