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中国物理学会期刊

基于石墨烯竖立片层常压相变制备纳米金刚石

CSTR: 32037.14.aps.73.20231064

Preparation of nanodiamonds based on phase transformation of vertical sheet under atmospheric pressure

CSTR: 32037.14.aps.73.20231064
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  • 采用热丝化学气相沉积法制备了含有钽原子的石墨烯竖立片层, 并将其置于含氧环境中进行退火处理, 在常压环境中发生相变得到纳米金刚石, 并研究退火环境中氧含量变化对纳米金刚石形成的影响. 结果表明, 当退火环境气压为10 Pa和50 Pa (对应氧原子百分比为1.96%和2.04%) 时, 退火后样品形貌与结构和未处理的石墨烯片层无异; 样品100 Pa和500 Pa气压下退火后(对应氧原子百分比为2.77%和3.11%), 在其中观察到了尺寸为2—4 nm的纳米金刚石, 这些金刚石晶粒多分布于非晶碳中; 继续升高退火环境气压则发现退火后样品被大面积氧化, 石墨结构遭到严重破坏. 该研究结果为纳米金刚石的制备提供了新方法.

     

    A basic and important way to prepare diamond is to make graphite experience the phase transformation under the high-pressure high-temperature (HPHT) condition. However, this method needs stringent equipment and high investment cost. Recently, we proposed a method to prepare the diamond by phase transformation of graphite at atmospheric pressure with monodispersed Ta atoms. It is found that a phase transformation happens to H atoms under atmospheric pressure, but the role of O atoms has not been investigated. Here, we use tantalum wires as Ta source and heat the filaments to prepare vertical graphene containing Ta atoms in hot filament chemical vapor deposition (HFCVD) system. And then the vertical graphene layers are annealed in oxygen-containing environment, and nanodiamonds are obtained by phase transformation from the vertical graphene under atmospheric pressure. The results show that the sample morphologies are the same as the untreated vertical graphene’s, when the annealed ambient air pressure is at 10 Pa and 50 Pa with oxygen atom content of 1.96% and 2.04%, respectively; TEM tests reveal TaC and graphite but no diamond in these samples . Nanodiamond grains with the size range of 2–4 nm are observed in the amorphous carbon region of samples annealed at 100 Pa and 500 Pa air pressure with oxygen atom content increasing to 2.77% and 3.11%, respectively, indicating that oxidation facilitates the phase change from Ta-containing vertical graphene to diamond at atmospheric pressure. When the air pressure of the annealing environment rises to 1000 Pa with the oxygen atom content of 3.54%, the sample is extensively oxidized and the graphite structure is severely damaged,which means that a large number of oxygen atoms tend to disrupt the graphite structure rather than promote the phase change into diamond. These results supply a way to prepare nanodiamond and show the effect of O atoms in the graphite phase transition at atmospheric pressure.

     

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