爆轰灰中sp3/sp2碳比调控与性能研究

Research on Regulation and Characterization of sp3/sp2 Carbon Ratio in Detonation Soot

  • 摘要: 纳米碳的sp3/sp2碳比对其催化性能、导电性、生物相容性等性能及应用有重要影响.本文借助高氯酸对爆轰灰中sp3/sp2碳比进行调控,对纯化后的爆轰灰(purified detonation soot, PDS)的元素组成、物相构成、sp3/sp2碳比进行表征,制备具有不同sp3/sp2碳比的爆轰灰负载金属钌催化剂(Ru/PDS),探究Ru/PDS在苯二甲酸二甲酯(DMT)加氢制备1,4-环己烷二甲酸二甲酯(DMCD)的反应中的催化性能.结果表明:纯化后的爆轰灰较为纯净,主要物质是纳米金刚石为核心多层石墨烯为壳的纳米碳结构,sp3/sp2比值范围为0.991~1.483,IDia/IG比值范围为0.447~0.856.DMT转化率最高可达66.67%,DMCD选择性均在81.93%以上,研究发现金属−载体相互作用是影响DMT转化率的重要因素. 具有不同sp3/sp2碳比的爆轰灰将在工业催化、含能材料燃烧性能调节和润滑油改性方面具有广阔的发展前景.

     

    Abstract: The sp3/sp2 carbon ratio of nanocarbon has an important effect on its catalytic property, electrical conductivity, biocompatibility and other properties and its applications. In this paper, the sp3/sp2 carbon ratio in the detonation soot was regulated by perchloric acid. The elemental composition, phase composition, and sp3/sp2 carbon ratio of the purified detonation soot (PDS) were characterized. Ruthenium (Ru) catalysts supported by PDS (Ru/PDS) with different sp3/sp2 carbon ratios were prepared to investigate the catalytic performance of Ru/PDS in the hydrogenation of dimethyl terephthalate (DMT) to dimethyl 1,4-cyclohexanedicarboxylate (DMCD). The results showed that the PDS was relatively pure, and the main component was nano carbon structure with nanodiamond as core and multilayer graphene as shell. The range of sp3/sp2 ratio was 0.991~1.483, and the range of IDia/IG was 0.447~0.856. The DMT conversion was up to 66.67% and the DMCD selectivity was above 81.93%. It is found that metal-support interaction is an important factor affecting DMT conversion. Detonation soot with different sp3/sp2 carbon ratios will have a broad development prospect in industrial catalysis, combustion performance regulation of energetic materials and modification of lubricating oil.

     

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