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通过自组装方法合成的具有特殊高有机含量的异常铜钴/氧化石墨烯复合材料:含能材料的热解与催化分解

Unusual Cu-Co/GO Composite with Special High Organic Content Synthesized by an Self-Assembly Approach: Pyrolysis and Catalytic Decomposition on Energetic Materials.

作者信息

Wang Jingjing, Lian Xiaoyan, Yan Qilong, Gao Dayuan, Zhao Fengqi, Xu Kangzhen

机构信息

School of Chemical Engineering/Integrated Military-Civilian Research Center for Energetic Materials, Northwest University, Xi'an 710069, China.

Science and Technology on Combustion, Internal Flow and Thermostructure Laboratory, Northwestern Polytechnical University, Xi'an 710072, China.

出版信息

ACS Appl Mater Interfaces. 2020 Jun 24;12(25):28496-28509. doi: 10.1021/acsami.0c05298. Epub 2020 Jun 9.

Abstract

An interesting Cu-Co/GO composite with special high organic content was accidentally fabricated for the first time via a one-pot solvothermal method in the mixed solvent of isopropanol and glycerol. The Cu-Co/GO composite was calcined separately in three different atmospheres (air, nitrogen, and argon) and further investigated by a series of characterization techniques. The results indicate that the spinel phase nano-CuCoO composite, nanometal oxides (CuO and CoO), and nanometal mixture of Cu and Co were unexpectedly formed after calcination in air, N, and Ar atmospheres, respectively, and the possible reaction mechanism was discussed. The specific mass losses of the Cu-Co/GO composite calcined in air, N, and Ar atmospheres were 28.14 %, 21.68 %, and 23.76 %, respectively. The catalytic decomposition performances of the as-prepared samples for cyclotrimethylenetrinitramine (RDX) and the mixture of nitrocellulose (NC) and RDX (NC + RDX) were investigated and compared via DSC method, and the results demonstrate that Cu-Co/GO composites obviously decrease the thermal decomposition temperature of RDX from 242.3 to 236.5 (before calcination), 238.6 (air), 235.8 (N), and 228.6 °C (Ar), respectively. Cu-Co/GO(Ar) composite exhibits the best catalytic decomposition performance among all samples, which makes the decomposition temperature of RDX and NC + RDX decrease by 13.7 and 4.9 °C and the apparent activation energy of decomposition for RDX decrease by 110.1 kJ/mol. The enhanced catalytic performance of Cu-Co/GO(Ar) composite could be attributed to the smaller particle size, better crystallinity, and specific well-dispersed metal atoms, whereas the Cu-Co/GO(air) composite after air calcination presents a bad catalytic performance due to the removal of GO.

摘要

首次通过一锅法溶剂热法在异丙醇和甘油的混合溶剂中意外制备了一种具有特殊高有机含量的有趣的铜钴/氧化石墨烯(Cu-Co/GO)复合材料。将Cu-Co/GO复合材料分别在三种不同气氛(空气、氮气和氩气)中煅烧,并通过一系列表征技术进行进一步研究。结果表明,分别在空气、氮气和氩气气氛中煅烧后,意外地形成了尖晶石相纳米CuCoO复合材料、纳米金属氧化物(CuO和CoO)以及Cu和Co的纳米金属混合物,并讨论了可能的反应机理。在空气、氮气和氩气气氛中煅烧的Cu-Co/GO复合材料的具体质量损失分别为28.14%、21.68%和23.76%。通过差示扫描量热法(DSC)研究并比较了所制备样品对环三亚甲基三硝胺(RDX)以及硝化纤维素(NC)和RDX混合物(NC + RDX)的催化分解性能,结果表明,Cu-Co/GO复合材料明显降低了RDX的热分解温度,从242.3℃分别降至236.5℃(煅烧前)、238.6℃(空气)、235.8℃(氮气)和228.6℃(氩气)。Cu-Co/GO(氩气)复合材料在所有样品中表现出最佳的催化分解性能,使RDX和NC + RDX的分解温度分别降低了13.7℃和4.9℃,并且RDX分解的表观活化能降低了110.1 kJ/mol。Cu-Co/GO(氩气)复合材料催化性能的增强可归因于较小的粒径、更好的结晶度以及特定的良好分散的金属原子,而空气煅烧后的Cu-Co/GO(空气)复合材料由于氧化石墨烯的去除而呈现出较差的催化性能。

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