Kinetics analysis of thermal decomposition of ammonium dinitramide (ADN)

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• 作者：Yu-ichiro Izato ; Mitsuo Koshi ; Atsumi Miyake…
• 关键词：Ammonium dinitramide ; Thermal decomposition ; Kinetics analysis ; TG ; DTA–MS–IR ; Ab initio calculation
• 刊名：Journal of Thermal Analysis and Calorimetry
• 出版年：2017
• 出版时间：January 2017
• 年：2017
• 卷：127
• 期：1
• 页码：255-264
• 全文大小：
• 刊物类别：Chemistry and Materials Science
• 刊物主题：Physical Chemistry; Analytical Chemistry; Polymer Sciences; Inorganic Chemistry; Measurement Science and Instrumentation;
• 出版者：Springer Netherlands
• ISSN：1588-2926
• 卷排序：127

文摘

Kinetics analyses were performed on the thermal decomposition of ammonium dinitramide (ADN) using thermogravimetry-differential thermal analysis–mass spectrometry–infrared spectroscopy (TG-DTA–MS–IR). The main evolved gases were determined to be NH₃, H₂O, N₂, NO, N₂O, and NO₂. The apparent activation energies of the exothermic, mass-change and gas-evolving reactions were analyzed on the basis of Friedman methods. The apparent activation energy of evolving N₂ has the same value as that of evolving H₂O since they occur by the same mechanism. A Friedman plot obtained from the DTA data has a curve similar to those obtained from N₂ and H₂O. The reaction that generated N₂ and H₂O plays an important role in the exothermic reaction in the decomposition of ADN. The activation energy for the N₂O evolution reaction has a range of approximately 120–152 kJ mol−1 with reaction progress values between 0.1 and 0.9. Quantum chemistry calculations revealed that the total energy barrier of dinitramic acid unimolecular decomposition and ammonium-dinitramic ions collision-induced decomposition is 149.9–156.0 and 160.6 kJ mol−1, respectively. These values are reasonable compared with the experimental value of 152 kJ mol−1.