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Growth of Single-Layer and Multilayer Graphene on Cu/Ni Alloy Substrates.
Accounts of Chemical Research ( IF 16.4 ) Pub Date : 2020-03-24 , DOI: 10.1021/acs.accounts.9b00643 Ming Huang 1, 2 , Rodney S Ruoff 1, 2, 3, 4
Accounts of Chemical Research ( IF 16.4 ) Pub Date : 2020-03-24 , DOI: 10.1021/acs.accounts.9b00643 Ming Huang 1, 2 , Rodney S Ruoff 1, 2, 3, 4
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ConspectusGraphene, a one-atom-thick layer of carbon with a honeycomb lattice, has drawn great attention due to its outstanding properties and its various applications in electronic and photonic devices. Mechanical exfoliation has been used for preparing graphene flakes (from monolayer to multilayer with thick pieces also typically present), but with sizes limited typically to less than millimeters, its usefulness is limited. Chemical vapor deposition (CVD) has been shown to be the most effective technique for the scalable preparation of graphene films with high quality and uniformity. To date, CVD growth of graphene on the most commonly used substrates (Cu and Ni foils) has been demonstrated and intensively studied. However, a survey of the existing literature and earlier work using Cu or Ni substrates for CVD growth indicates that the bilayer and multilayer graphene over a large area, particularly single crystals, have not been obtained.In this Account, we review current progress and development in the CVD growth of graphene and highlight the important challenges that need to be addressed, for example, how to achieve large single crystal graphene films with a controlled number of layers. A single-layer graphene film grown on polycrystalline Cu foil was first reported by our group, and since then various techniques have been devoted to achieving the fast growth of large-area graphene films with high quality. Commercially available Cu/Ni foils, sputtered Cu/Ni thin films, and polycrystalline Cu/Ni foils have been used for the CVD synthesis of bilayer, trilayer, and multilayer graphene. Cu/Ni alloy substrates are particularly interesting due to their greater carbon solubility than pure Cu substrates and this solubility can be finely controlled by changing the alloy composition. These substrates with controlled compositions have shown the potential for the growth of layer-tunable graphene films in addition to providing a much higher growth rate due to their stronger catalytic activity. However, the well-controlled preparation of single crystal graphene with a defined number of layers on Cu/Ni substrates is still challenging.Due to its small lattice mismatch with graphene, a single crystal Cu(111) foil has been shown to be an ideal substrate for the epitaxial growth of graphene. Our group has reported the synthesis of large-size single crystal Cu(111) foils by the contact-free annealing of commercial Cu foils, and single crystal Cu/Ni(111) alloy foils have also been obtained after the heat-treatment of Ni-coated Cu(111) foils. The use of these single crystal foils (especially the Cu/Ni alloy foils) as growth substrates has enabled the fast growth of single crystal single-layer graphene films. By increase of the Ni content, single crystal bilayer, trilayer, and even multilayer graphene films have been synthesized. In addition, we also discuss the wafer-scale growth of single-layer graphene on the single crystalline Cu/Ni(111) thin films.Recent research results on the large-scale preparation of single crystal graphene films with different numbers of layers on various types of Cu/Ni alloy substrates with different compositions are reviewed and discussed in detail. Despite the remarkable progress in this field, further challenges, such as the wafer-scale synthesis of single crystal graphene with a controlled number of layers and a deeper understanding of the growth mechanism of bilayer and multilayer graphene growth on Cu/Ni substrates, still need to be addressed.
中文翻译：
Cu / Ni合金基底上单层和多层石墨烯的生长。
石墨烯是具有蜂窝晶格的单原子厚的碳层，因其出色的性能以及在电子和光子设备中的各种应用而备受关注。机械剥离已用于制备石墨烯薄片（从单层到通常也有厚片的多层），但是尺寸通常限制为小于毫米，因此其用途受到限制。化学气相沉积（CVD）已被证明是可缩放制备高质量和均匀性石墨烯薄膜的最有效技术。迄今为止，已经证明并深入研究了石墨烯在最常用的衬底（铜和镍箔）上的CVD生长。然而，对现有文献和使用Cu或Ni衬底进行CVD生长的早期工作的调查表明，尚未获得大面积的双层和多层石墨烯，特别是单晶。石墨烯的CVD生长并突出了需要解决的重要挑战，例如，如何实现具有受控层数的大型单晶石墨烯薄膜。我们的小组首次报道了在多晶铜箔上生长的单层石墨烯薄膜，从那时起，各种技术致力于实现高质量的大面积石墨烯薄膜的快速生长。商购的Cu / Ni箔，溅射Cu / Ni薄膜和多晶Cu / Ni箔已用于CVD双层，三层，和多层石墨烯。Cu / Ni合金基材比纯Cu基材具有更高的碳溶解度，因此特别令人感兴趣，并且可以通过更改合金成分来精细控制此溶解度。这些具有受控组成的基材由于其更强的催化活性，除了提供更高的生长速率外，还显示了可层可调石墨烯薄膜生长的潜力。然而，在Cu / Ni衬底上以可控的方式制备具有一定层数的单晶石墨烯仍然具有挑战性。由于单晶石墨烯与石墨烯的晶格失配较小，因此单晶Cu（111）箔已被证明是理想的选择石墨烯外延生长的衬底。我们的小组已经报道了通过商用铜箔的无接触退火来合成大尺寸单晶Cu（111）箔，并且在对Ni进行热处理之后也获得了单晶Cu / Ni（111）合金箔。涂层的Cu（111）箔。这些单晶箔（特别是Cu / Ni合金箔）用作生长衬底使得单晶单层石墨烯膜能够快速生长。通过增加Ni含量，已经合成了单晶双层，三层甚至多层石墨烯膜。此外，我们还讨论了单晶Cu / Ni（111）薄膜上单层石墨烯的晶圆级生长。综述并详细讨论了在各种类型的具有不同组成的Cu / Ni合金衬底上大规模制备具有不同层数的单晶石墨烯薄膜的最新研究成果。尽管在该领域取得了长足的进步，但仍需要进一步的挑战，例如以晶圆级合成具有可控层数的单晶石墨烯，以及对Cu / Ni衬底上双层和多层石墨烯生长的生长机理有更深入的了解待解决。
更新日期：2020-04-23
中文翻译：
Cu / Ni合金基底上单层和多层石墨烯的生长。
石墨烯是具有蜂窝晶格的单原子厚的碳层，因其出色的性能以及在电子和光子设备中的各种应用而备受关注。机械剥离已用于制备石墨烯薄片（从单层到通常也有厚片的多层），但是尺寸通常限制为小于毫米，因此其用途受到限制。化学气相沉积（CVD）已被证明是可缩放制备高质量和均匀性石墨烯薄膜的最有效技术。迄今为止，已经证明并深入研究了石墨烯在最常用的衬底（铜和镍箔）上的CVD生长。然而，对现有文献和使用Cu或Ni衬底进行CVD生长的早期工作的调查表明，尚未获得大面积的双层和多层石墨烯，特别是单晶。石墨烯的CVD生长并突出了需要解决的重要挑战，例如，如何实现具有受控层数的大型单晶石墨烯薄膜。我们的小组首次报道了在多晶铜箔上生长的单层石墨烯薄膜，从那时起，各种技术致力于实现高质量的大面积石墨烯薄膜的快速生长。商购的Cu / Ni箔，溅射Cu / Ni薄膜和多晶Cu / Ni箔已用于CVD双层，三层，和多层石墨烯。Cu / Ni合金基材比纯Cu基材具有更高的碳溶解度，因此特别令人感兴趣，并且可以通过更改合金成分来精细控制此溶解度。这些具有受控组成的基材由于其更强的催化活性，除了提供更高的生长速率外，还显示了可层可调石墨烯薄膜生长的潜力。然而，在Cu / Ni衬底上以可控的方式制备具有一定层数的单晶石墨烯仍然具有挑战性。由于单晶石墨烯与石墨烯的晶格失配较小，因此单晶Cu（111）箔已被证明是理想的选择石墨烯外延生长的衬底。我们的小组已经报道了通过商用铜箔的无接触退火来合成大尺寸单晶Cu（111）箔，并且在对Ni进行热处理之后也获得了单晶Cu / Ni（111）合金箔。涂层的Cu（111）箔。这些单晶箔（特别是Cu / Ni合金箔）用作生长衬底使得单晶单层石墨烯膜能够快速生长。通过增加Ni含量，已经合成了单晶双层，三层甚至多层石墨烯膜。此外，我们还讨论了单晶Cu / Ni（111）薄膜上单层石墨烯的晶圆级生长。综述并详细讨论了在各种类型的具有不同组成的Cu / Ni合金衬底上大规模制备具有不同层数的单晶石墨烯薄膜的最新研究成果。尽管在该领域取得了长足的进步，但仍需要进一步的挑战，例如以晶圆级合成具有可控层数的单晶石墨烯，以及对Cu / Ni衬底上双层和多层石墨烯生长的生长机理有更深入的了解待解决。
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