石墨烯催化生长中的偏析现象及其调控方法

doi:10.6023/A13010023

摘要/Abstract

石墨烯是一种由sp²杂化碳原子组成的具有蜂窝状结构的二维原子晶体, 其一系列优异的电学、光学和力学等特性, 使得它在各领域都有广泛的应用前景, 而大面积高质量石墨烯的制备则是各类应用的前提. 金属基底上的催化生长方法是目前制备高质量石墨烯的主流技术. 系统地阐释了金属基底上石墨烯催化生长中的偏析现象以及我们发展的通过调控偏析过程来实现石墨烯控制生长的基本方法. 这些方法包括: 偏析生长法、共偏析法、Cu-Ni合金偏析法、互补性二元合金催化法等. 我们的工作表明, 偏析是金属表面石墨烯生长过程中无法回避的、同时也可以积极利用的一个关键基元步骤. 对偏析现象及其调控方法的研究, 有助于为石墨烯的控制生长提供新的解决方案, 进而推动石墨烯的工业化进程.

关键词: 石墨烯, 偏析现象, 平衡偏析与非平衡偏析, 化学气相沉积, 层数控制, 掺杂控制

Graphene, a sp²-hybridized two-dimensional honeycomb structure of carbon, has attracted great attentions because of its excellent electrical, optical and mechanical properties. One of the major challenges for its various applications is the production of large-area and high-quality graphene. Among the typical approaches reported up to now, catalytic growth on metal surfaces has become the most attractive technique for graphene synthesis with high quality. Segregation, which refers to the enrichment of carbon onto the surface of metals, is one of the key elementary steps for the catalytic growth of graphene on metal surface. In this paper, we will systematically study the segregation phenomenon and the possibility of its control for graphene growth. We will also demonstrate the typical approaches we have developed for growing high-quality graphene by designing and controlling the segregation process, which include segregation technique, co-segregation, synergistic bimetal alloy technique, etc. For instance, with a designed binary alloy, such as Ni/Mo, Co/Mo, or Fe/Mo, we effectively suppressed the carbon precipitation step and achieved perfect single layer graphene with 100% surface coverage by chemical vapor deposition method. With a segregation-only process of carbon atoms predissolved in bulk metals such as Ni, Co, Ni-Cu alloy and Fe, we succeeded in growing wafer-scale high-quality graphene without using extraneous carbon sources. Using co-segregation technique, we could directly grow nitrogen-doped graphene on nickel with controlled dopant concentration and spatial location. These studies will greatly help to understand the catalytic growth process of graphene and further promote its practical applications.

Key words: graphene, segregation phenomenon, equilibrium and non-equilibrium segregation, chemical vapor deposition, layer control, doping control

引用此文

张朝华, 付磊, 张艳锋, 刘忠范. 石墨烯催化生长中的偏析现象及其调控方法[J]. 化学学报, 2013, 71(03): 308-322.

Zhang Chaohua, Fu Lei, Zhang Yanfeng, Liu Zhongfan. Segregation Phenomenon and Its Control in the Catalytic Growth of Graphene[J]. Acta Chimica Sinica, 2013, 71(03): 308-322.

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