Center for Nanochemistry (CNC), College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.
State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.
Adv Mater. 2017 Aug;29(32). doi: 10.1002/adma.201701325. Epub 2017 Jun 20.
The direct growth of high-quality, large-area, uniform, vertically stacked Gr/h-BN heterostructures is of vital importance for applications in electronics and optoelectronics. However, the main challenge lies in the catalytically inert nature of the hexagonal boron nitride (h-BN) substrates, which usually afford a rather low decomposition rate of carbon precursors, and thus relatively low growth rate of graphene. Herein, a nickelocene-precursor-facilitated route is developed for the fast growth of Gr/h-BN vertical heterostructures on Cu foils, which shows much improved synthesis efficiency (8-10 times faster) and crystalline quality of graphene (large single-crystalline domain up to ≈20 µm). The key advantage of our synthetic route is the utilization of nickel atoms that are decomposed from nickelocene molecules as the gaseous catalyst, which can decrease the energy barrier for graphene growth and facilitate the decomposition of carbon sources, according to our density functional theory calculations. The high-quality Gr/h-BN stacks are proved to be perfect anode/protecting layers for high-performance organic light-emitting diode devices. In this regard, this work offers a brand-new route for the fast growth of Gr/h-BN heterostructures with practical scalability and high crystalline quality, thus should propel its wide applications in transparent electrodes, high-performance electronic devices, and energy harvesting/transition directions.
高质量、大面积、均匀、垂直堆叠的 Gr/h-BN 异质结构的直接生长对于电子学和光电学的应用至关重要。然而,主要的挑战在于六方氮化硼(h-BN)衬底的催化惰性,这通常导致碳前体的分解率较低,因此石墨烯的生长速度相对较低。在此,我们开发了一种利用环戊二烯镍前体制备 Gr/h-BN 垂直异质结构的方法,该方法在 Cu 箔上快速生长 Gr/h-BN 垂直异质结构,具有更高的合成效率(快 8-10 倍)和更高的石墨烯晶体质量(大单晶畴可达约 20 µm)。我们的合成路线的关键优势是利用环戊二烯镍分子分解产生的镍原子作为气态催化剂,根据我们的密度泛函理论计算,这可以降低石墨烯生长的能垒并促进碳源的分解。高质量的 Gr/h-BN 堆叠被证明是高性能有机发光二极管器件的理想阳极/保护层。在这方面,这项工作为具有实际可扩展性和高晶体质量的 Gr/h-BN 异质结构的快速生长提供了一条全新的途径,从而应该推动其在透明电极、高性能电子器件和能量收集/转换方向的广泛应用。