Layer-by-layer growth of bilayer graphene single-crystals enabled by proximity catalytic activity

IF 13.2 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
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Abstract

Direct growth of large-area vertically stacked two-dimensional (2D) van der Waal (vdW) materials is a prerequisite for their high-end applications in integrated electronics, optoelectronics and photovoltaics. Currently, centimetre- to even metre-scale monolayers of single-crystal graphene (MLG) and hexagonal boron nitride (h-BN) have been achieved by epitaxial growth on various single-crystalline substrates. However, in principle, this success in monolayer epitaxy seems extremely difficult to be replicated to bi- or few-layer growth, as the full coverage of the first layer was believed to terminate the reactivity of those adopting catalytic metal surfaces. Here, we report an exceptional layer-by-layer chemical vapour deposition (CVD) growth of large size bi-layer graphene single-crystals, enabled by proximity catalytic activity from platinum (Pt) surfaces to the outermost graphene layers. In-situ growth and real-time surveillance experiments, under well-controlled environments, unambiguously verify that the growth does follow the layer-by-layer mode on open surfaces of MLG/Pt(111). First-principles calculations indicate that the transmittal of catalytic activity is allowed by an appreciable electronic hybridisation between graphene overlayers and Pt surfaces, enabling catalytic dissociation of hydrocarbons and subsequently direct graphitisation of their radicals on the outermost sp2 carbon surface. This proximity catalytic activity is also proven to be robust for tube-furnace CVD in fabricating single-crystalline graphene bi-, tri- and tetra-layers, as well as h-BN few-layers. Our findings offer an exceptional strategy for potential controllable, layer-by-layer and wafer-scale growth of vertically stacked few-layered 2D single crystals.

通过近距离催化活性实现双层石墨烯单晶的逐层生长
直接生长大面积垂直堆叠的二维(2D)范德华(vdW)材料是其在集成电子、光电和光伏领域高端应用的先决条件。目前,单晶石墨烯(MLG)和六方氮化硼(h-BN)的厘米级甚至米级单层已通过在各种单晶基底上外延生长而实现。然而,从原理上讲,这种单层外延生长的成功似乎很难复制到双层或少层生长上,因为第一层的完全覆盖被认为会终止那些采用催化金属表面的反应性。在这里,我们报告了一种特殊的逐层化学气相沉积(CVD)生长大尺寸双层石墨烯单晶的方法,该方法通过铂(Pt)表面与最外层石墨烯的近距离催化活性来实现。在控制良好的环境下进行的原位生长和实时监控实验明确验证了在 MLG/Pt(111)开放表面上的生长确实遵循逐层模式。第一性原理计算表明,石墨烯覆盖层与铂表面之间明显的电子杂化使得催化活性得以传递,从而实现了碳氢化合物的催化解离,并随后在最外层的 sp2 碳表面直接将其自由基石墨化。事实证明,这种近距离催化活性在管式炉 CVD 制造单晶双层、三层和四层石墨烯以及 h-BN 少数层时也很有效。我们的研究结果为垂直堆叠少层二维单晶的潜在可控、逐层和晶圆级生长提供了一种特殊策略。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Nano Today
Nano Today 工程技术-材料科学:综合
CiteScore
21.50
自引率
3.40%
发文量
305
审稿时长
40 days
期刊介绍: Nano Today is a journal dedicated to publishing influential and innovative work in the field of nanoscience and technology. It covers a wide range of subject areas including biomaterials, materials chemistry, materials science, chemistry, bioengineering, biochemistry, genetics and molecular biology, engineering, and nanotechnology. The journal considers articles that inform readers about the latest research, breakthroughs, and topical issues in these fields. It provides comprehensive coverage through a mixture of peer-reviewed articles, research news, and information on key developments. Nano Today is abstracted and indexed in Science Citation Index, Ei Compendex, Embase, Scopus, and INSPEC.
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