Institute of Chemical Materials, China Academy of Engineering Physics , Mianyang 621900, China.
ACS Appl Mater Interfaces. 2017 Mar 29;9(12):10684-10691. doi: 10.1021/acsami.7b00287. Epub 2017 Mar 17.
High energy and low signature properties are the future trend of solid propellant development. As a new and promising oxidizer, hexanitrohexaazaisowurtzitane (CL-20) is expected to replace the conventional oxidizer ammonium perchlorate to reach above goals. However, the high pressure exponent of CL-20 hinders its application in solid propellants so that the development of effective catalysts to improve the thermal decomposition properties of CL-20 still remains challenging. Here, 3D hierarchically ordered porous carbon (3D HOPC) is presented as a catalyst for the thermal decomposition of CL-20 via synthesizing a series of nanostructured CL-20/HOPC composites. In these nanocomposites, CL-20 is homogeneously space-confined into the 3D HOPC scaffold as nanocrystals 9.2-26.5 nm in diameter. The effect of the pore textural parameters and surface modification of 3D HOPC as well as CL-20 loading amount on the thermal decomposition of CL-20 is discussed. A significant improvement of the thermal decomposition properties of CL-20 is achieved with remarkable decrease in decomposition peak temperature (from 247.0 to 174.8 °C) and activation energy (from 165.5 to 115.3 kJ/mol). The exceptional performance of 3D HOPC could be attributed to its well-connected 3D hierarchically ordered porous structure, high surface area, and the confined CL-20 nanocrystals. This work clearly demonstrates that 3D HOPC is a superior catalyst for CL-20 thermal decomposition and opens new potential for further applications of CL-20 in solid propellants.
高能低特征是固体推进剂发展的未来趋势。六硝基六氮杂异伍兹烷(CL-20)作为一种新型有前途的氧化剂,有望替代传统的氧化剂高氯酸铵来达到上述目标。然而,CL-20 的高压指数阻碍了其在固体推进剂中的应用,因此开发有效的催化剂来改善 CL-20 的热分解性能仍然具有挑战性。本文通过合成一系列纳米结构的 CL-20/HOPC 复合材料,提出了 3D 有序多孔碳(3D HOPC)作为 CL-20 热分解的催化剂。在这些纳米复合材料中,CL-20 均匀地空间限制在 3D HOPC 支架中,形成 9.2-26.5nm 直径的纳米晶体。讨论了 3D HOPC 的孔结构参数和表面改性以及 CL-20 负载量对 CL-20 热分解的影响。CL-20 的热分解性能得到显著改善,分解峰温度从 247.0℃显著降低至 174.8℃,活化能从 165.5kJ/mol 降低至 115.3kJ/mol。3D HOPC 的优异性能可归因于其良好连通的 3D 有序多孔结构、高比表面积和受限的 CL-20 纳米晶体。这项工作清楚地表明,3D HOPC 是 CL-20 热分解的优异催化剂,并为 CL-20 在固体推进剂中的进一步应用开辟了新的潜力。