Synthesis of nitrogen-containing carbon nanofibers by catalytic decomposition of ethylene/ammonia mixture
Synthesis of nitrogen-containing carbon nanofibers by catalytic decomposition of ethylene/ammonia mixture
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DOI：
10.1016/j.carbon.2007.04.032
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发表时间：
2007-08
期刊：
影响因子：
10.9
通讯作者：
A. E. Shalagina;Z. Ismagilov;O. Podyacheva;R. Kvon;V. Ushakov
中科院分区：
文献类型：
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作者：
A. E. Shalagina;Z. Ismagilov;O. Podyacheva;R. Kvon;V. Ushakov
在450-675°C下，研究了90 Ni-Al 2 O3，82 Ni-8 Cu-Al 2 O3，65 Ni-25 Cu-Al 2 O3，45 Ni-45 Cu-Al 2 O3，90 Fe-Al 2 O3，85 Fe-5Co-Al 2 O3，62 Fe-8 Co-Al 2 O3，62 Fe-8 Ni-Al 2 O3金属催化剂上乙炔/氨水混合物分解过程中氮掺杂碳纳米纤维（CNFs）的形成。结果发现，CNFs的产率，它们的结构和质地性质，以及CNFs中的氮含量强烈地依赖于合成条件，如：所使用的催化剂，进料组成，温度和持续时间。结果表明，65 Ni-25 Cu-Al 2 O3是制备含氮纳米碳纤维（N-CNFs）的最佳催化剂，其氮含量可达7 wt.%。进料中的氨浓度等于75体积%，结果表明，反应温度550°C，反应时间1h是N-CNFs中氮含量最高的反应条件。TEM研究表明，纳米纤维具有螺旋形态和由石墨片组成的“人字形”结构。根据XPS数据，N-CNF结构中的氮掺入导致形成两种类型的氮配位：吡啶和季铵，并且它们的丰度取决于反应条件。
The formation of carbon nanofibers (CNFs) doped with nitrogen was investigated during decomposition of C2H4/NH3mixtures at 450–675°C over metal catalysts: 90Ni–Al2O3, 82Ni–8Cu–Al2O3, 65Ni–25Cu–Al2O3, 45Ni–45Cu–Al2O3, 90Fe–Al2O3, 85Fe–5Co–Al2O3, 62Fe–8Co–Al2O3, 62Fe–8Ni–Al2O3. It was found that the yield of CNFs, their structural and textural properties, as well as nitrogen content in CNFs are strongly dependent on the synthesis conditions such as: catalyst used, feed composition, temperature and duration. The 65Ni–25Cu–Al2O3was proved to be the most efficient catalyst for the production of nitrogen-containing carbon nanofibers (N-CNFs) with nitrogen content up to 7wt.%. Ammonia concentration in the feed equal 75vol.%, temperature 550°C and duration 1h were found to be the optimum reaction parameters to reach the maximum nitrogen content in N-CNFs. TEM studies revealed that the nanofibers have a helical morphology and a “herringbone” structure composed of graphite sheets. According to the XPS data, the nitrogen incorporation in the N-CNF structure leads to the formation of two types of nitrogen coordination: pyridinic and quaternary, and their abundance depends on the reaction conditions.