New energetic nitroformate salts that contain high‐nitrogen cations were synthesized by taking advantage of the relatively high acidity of nitroform. All of the new salts have been characterized by elemental, spectral, and thermal analyses. Single‐crystal X‐ray analysis of 2 shows that it is a co‐crystal of a neutral 4‐amino‐1,2,4‐triazole molecule with the 4‐amino‐1,2,4‐triazolium nitroformate ion pair. The presence of the neutral molecule appears to lend stability to the salt. The structure of 3,6‐diguanidino‐1,2,4,5‐tetrazinium nitroformate ( 10 ) was also confirmed by single‐crystal X‐ray analysis. Theoretical performance calculations indicate that these materials have properties which compare favorably with hydrazinium nitroformate, TNT and Tetryl suggesting potential applications as eco‐friendly oxidizers. (© Wiley‐VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2007)
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