Evolution of ordered nanoporous phases during h-BN growth: controlling the route from gas-phase precursor to 2D material by in situ monitoring.
Evolution of ordered nanoporous phases during h-BN growth: controlling the route from gas-phase precursor to 2D material by in situ monitoring.
复制标题
h-BN生长过程中有序纳米孔相的演化：通过原位监测控制气相前驱体到二维材料的路径。
DOI：
10.1039/d2nh00353h
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发表时间：
2022-10-24
影响因子：
9.7
通讯作者：
中科院分区：
文献类型：
--
作者：
二维（2D）材料（例如石墨烯和六方氮化硼（h-BN））的大面积单晶单层可以通过化学气相沉积（CVD）来生长。然而，从气相前体到2D材料的转化出现的高温和快速时间尺度使得同时遵循原子排列极具挑战性。我们利用氦原子散射来发现和控制CVD过程中新型2D h-BN纳米多孔相的生长。我们发现，在气相前驱体形成h-BN之前，形成了亚稳（3 × 3）结构，并且在所得的2D h-BN上过量沉积导致出现（3 × 4）结构。我们说明，这些纳米多孔结构是通过吸附后的环硼氮烷前体的部分脱氢和聚合产生的。这些步骤在2D材料的合成过程中基本上未被探索，我们揭示了CVD生长过程中的丰富相。我们的研究结果为CVD中的2D材料工程提供了重要的基础，通过调整或仔细控制生长条件，从而利用这些中间结构合成共价自组装2D网络。在h-BN的生长之后的衍射测量揭示了在形成期间的中间远程有序的开放网络结构。DFT计算解释了它们的性质，概述了控制共价2D网络合成的新途径。
Large-area single-crystal monolayers of two-dimensional (2D) materials such as graphene and hexagonal boron nitride (h-BN) can be grown by chemical vapour deposition (CVD). However, the high temperatures and fast timescales at which the conversion from a gas-phase precursor to the 2D material appears, make it extremely challenging to simultaneously follow the atomic arrangements. We utilise helium atom scattering to discover and control the growth of novel 2D h-BN nanoporous phases during the CVD process. We find that prior to the formation of h-BN from the gas-phase precursor, a metastable (3 × 3) structure is formed, and that excess deposition on the resulting 2D h-BN leads to the emergence of a (3 × 4) structure. We illustrate that these nanoporous structures are produced by partial dehydrogenation and polymerisation of the borazine precursor upon adsorption. These steps are largely unexplored during the synthesis of 2D materials and we unveil the rich phases during CVD growth. Our results provide significant foundations for 2D materials engineering in CVD, by adjusting or carefully controlling the growth conditions and thus exploiting these intermediate structures for the synthesis of covalent self-assembled 2D networks. Diffraction measurements following the growth of h-BN, reveal intermediate long-range ordered open network structures during the formation. DFT calculations explain their nature, outlining new routes to control the synthesis of covalent 2D networks.
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影响因子：
3.9
作者：
Anemone, Gloria;Climent-Pascual, Esteban;Farias, Daniel
通讯作者：
Farias, Daniel
影响因子：
2.9
作者：
Avidor, N.;Hedgeland, H.;Alexandrowicz, G.
通讯作者：
Alexandrowicz, G.
影响因子：
3.3
作者：
Borca, Bogdana;Barja, Sara;Miranda, Rodolfo
通讯作者：
Miranda, Rodolfo
影响因子：
8.6
作者：
Chen, Hua;Zhu, Wenguang;Zhang, Zhenyu
通讯作者：
Zhang, Zhenyu
影响因子：
5.7
作者：
Avidor, N.;Allison, W.
通讯作者：
Allison, W.