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首页> 外文期刊>RSC Advances >Bottom-up design of high-energy-density molecules (N2CO)n (n = 2–8)
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Bottom-up design of high-energy-density molecules (N2CO)n (n = 2–8)

机译：高能密度分子（N 2 CO） n （ n = 2– 8）

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Seeking high-energy-density materials (HEDMs) with balanced huge energy release and good stability has remained quite a tough task for both experimentalists and theoreticians. The current HEDM design mostly concentrates on the chemical modification of either the skeletons or ligands. To increase the number of HEDM candidates, a novel design strategy is highly desired. In this paper, we computationally proposed a bottom-up strategy, i.e., a suitable HEDM seed (e.g., cyc-N2CO) can form novel HEDMs while retaining good stability and good performance. Starting from the experimentally known diazirinone (cyc-N2CO) as a “seed” and by considering various bond-addition channels (2 + 2/2 + 3/3 + 3 cyclo-addition at the NN/CO/C–N bonds), we found that the cyc-N2CO dimer isomer 1 (i.e., (N2CO)2 containing a COCO ring with an exocyclic side-N2 at each C-atom) possess the rate-determining barrier of 29.9 kcal mol?1 and exothermicity of 168.7 kcal mol?1 into 2N2 + 2CO at the composite CBS-QB3 level. Moreover, the trimer and tetramer of cyc-N2CO each possess high rate-determining barriers of 25.8 and 30.3 kcal mol?1, respectively, at the CBS-QB3 level. Even higher oligomers with n = 5–8 have rate-determining barriers around 25 and 34 kcal mol?1. The spiral skeletons were shown to have a contribution to their good inherent kinetic stability. By comparing the detonation properties with some known HEDM compounds, the oligomers of cyc-N2CO may well deserve future synthetic trials for novel HEDMs. Our designed (N2CO)n with all the untouched NN bonds differed sharply from the recently reported high-pressure polymerized forms, in which all the double bonds have been transformed into single bonds. The present bottom-up strategy from an HEDM seed (i.e., cyc-N2CO) to novel oligomeric HEDMs confirmed by the CBS-QB3 calculations seems to be quite promising and may open a new way of designing in the HEDM realm.
机译：寻求具有平衡的巨大能量释放和良好稳定性的高能量密度材料（HEDM），对于实验家和理论家而言仍然是一项艰巨的任务。当前的HEDM设计主要集中在骨架或配体的化学修饰上。为了增加HEDM候选者的数量，非常需要一种新颖的设计策略。在本文中，我们通过计算提出了一种自下而上的策略，即 ie ，一种合适的HEDM种子（ eg ， cyc -N < sub> 2 CO）可以形成新型HEDM，同时保持良好的稳定性和良好的性能。从实验已知的重氮基酮（ cyc -N 2 CO）作为“种子”开始，并考虑各种键加通道（2 +在NN / CO / C–N键上2/2 + 3/3 + 3个环加成），我们发现 cyc -N 2 < / small> CO二聚体异构体1（ ie ，（N 2 CO） 2 在每个C原子上带有一个环外侧为N 2 的COCO环）具有29.9 kcal mol ？1 ，放热为168.7 kcal mol ？1 到2N 2 + 2CO复合CBS-QB3级。此外， cyc -N 2 CO的三聚体和四聚体均具有较高的速率测定势垒，分别为25.8和30.3 kcal mol <在CBS-QB3级别分别为sup>？1 。 n = 5–8的甚至更高的低聚物在25和34 kcal mol ？1 左右具有速率决定性势垒。螺旋骨架显示出对其良好的固有动力学稳定性的贡献。通过与一些已知的HEDM化合物比较其爆炸特性，cyc-N 2 CO的低聚物可能值得为新型HEDM进行未来的合成试验。我们设计的（N 2 CO） n ，所有未接触的NN键都不同与最近报道的高压聚合形式截然不同，在高压聚合形式中，所有双键都已转变为单键。从HEDM种子（ ie ， cyc -N 2 CO）当前的自下而上策略通过CBS-QB3计算确认的HEDM似乎很有前途，并可能为HEDM领域开辟一种新的设计方式。

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