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    In Situ Fabrication of Freestanding Single-Atom-Thick 2D Metal/Metallene and 2D Metal/ Metallene Oxide Membranes: Recent Developments
    (Weinheim : Wiley-VCH, 2021) Ta, Huy Q.; Mendes, Rafael G.; Liu, Yu; Yang, Xiaoqin; Luo, Jingping; Bachmatiuk, Alicja; Gemming, Thomas; Zeng, Mengqi; Fu, Lei; Liu, Lijun; Rümmeli, Mark H.
    In recent years, two-dimensional (2D) materials have attracted a lot of research interest as they exhibit several fascinating properties. However, outside of 2D materials derived from van der Waals layered bulk materials only a few other such materials are realized, and it remains difficult to confirm their 2D freestanding structure. Despite that, many metals are predicted to exist as 2D systems. In this review, the authors summarize the recent progress made in the synthesis and characterization of these 2D metals, so called metallenes, and their oxide forms, metallene oxides as free standing 2D structures formed in situ through the use of transmission electron microscopy (TEM) and scanning TEM (STEM) to synthesize these materials. Two primary approaches for forming freestanding monoatomic metallic membranes are identified. In the first, graphene pores as a means to suspend the metallene or metallene oxide and in the second, electron-beam sputtering for the selective etching of metal alloys or thick complex initial materials is employed to obtain freestanding single-atom-thick 2D metal. The data show a growing number of 2D metals/metallenes and 2D metal/ metallene oxides having been confirmed and point to a bright future for further discoveries of these 2D materials.
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    Advances and Trends in Chemically Doped Graphene
    (Weinheim : Wiley-VCH, 2020) Ullah, Sami; Shi, Qitao; Zhou, Junhua; Yang, Xiaoqin; Ta, Huy Q.; Hasan, Maria; Ahmad, Nasir Mahmood; Fu, Lei; Bachmatiuk, Alicja; Rümmeli, Mark H.
    Chemically doped graphene materials are fascinating because these have different desirable attributes with possible synergy. The inert and gapless nature of graphene can be changed by adding a small number of heteroatoms to substitute carbon in the lattice. The doped material may display superior catalytic activities; durable, fast, and selective sensing; improved magnetic moments; photoresponses; and activity in chemical reactions. In the current review, recent advances are covered in chemically doped graphene. First, the different types of heteroatoms, their bonding configurations, and briefly their properties are discussed. This is followed by the description of various synthesis and analytical methods essential for assessing the characteristics of heterographene with specific focus on the selected graphene materials of different dopants (particularly, single dopants, including N, B, S, P, first three halogens, Ge, and Ga, and codopants, such as N/O), and more importantly, up-to-date applications enabled by the intentional doping. Finally, outlook and perspectives section review the existing challenges, future opportunities, and possible ways to improve the graphitic materials. The goal is to update and inspire the readers to establish novel doped graphene with valuable properties and for current and futuristic applications. © 2020 The Authors. Published by Wiley-VCH GmbH
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    On the Catalytic Activity of Sn Monomers and Dimers at Graphene Edges and the Synchronized Edge Dependence of Diffusing Atoms in Sn Dimers
    (Weinheim : Wiley-VCH, 2021) Yang, Xiaoqin; Ta, Huy Q.; Hu, Huimin; Liu, Shuyuan; Liu, Yu; Bachmatiuk, Alicja; Luo, Jinping; Liu, Lijun; Choi, Jin-Ho; Rummeli, Mark H.
    In this study, in situ transmission electron microscopy is performed to study the interaction between single (monomer) and paired (dimer) Sn atoms at graphene edges. The results reveal that a single Sn atom can catalyze both the growth and etching of graphene by the addition and removal of C atoms respectively. Additionally, the frequencies of the energetically favorable configurations of an Sn atom at a graphene edge, calculated using density functional theory calculations, are compared with experimental observations and are found to be in good agreement. The remarkable dynamic processes of binary atoms (dimers) are also investigated and is the first such study to the best of the knowledge. Dimer diffusion along the graphene edges depends on the graphene edge termination. Atom pairs (dimers) involving an armchair configuration tend to diffuse with a synchronized shuffling (step-wise shift) action, while dimer diffusion at zigzag edge terminations show a strong propensity to collapse the dimer with each atom diffusing in opposite directions (monomer formation). Moreover, the data reveals the role of C feedstock availability on the choice a single Sn atom makes in terms of graphene growth or etching. This study advances the understanding single atom catalytic activity at graphene edges. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
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    In Situ Observations of Freestanding Single-Atom-Thick Gold Nanoribbons Suspended in Graphene
    (Weinheim : Wiley-VCH, 2020) Zhao, Liang; Ta, Huy Q.; Mendes, Rafael G.; Bachmatiuk, Alicja; Rummeli, Mark H.
    Bulk gold's attributes of relative chemical inertness, rarity, relatively low melting point and its beautiful sheen make it a prized material for humans. Recordings suggest it was the first metal employed by humans dating as far back to the late Paleolithic period ≈40 000 BC. However, at the nanoscale gold is expected to present new and exciting properties, not least in catalysis. Moreover, recent studies suggest a new family of single-atom-thick two-dimensional (2D) metals exist. This work shows single-atom-thick freestanding gold membranes and nanoribbons can form as suspended structures in graphene pores. Electron irradiation is shown to lead to changes to the graphene pores which lead to dynamic changes of the gold membranes which transition to a nanoribbon. The freestanding single-atom-thick 2D gold structures are relatively stable to electron irradiation for extended periods. The work should advance the development of 2D gold monolayers significantly. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim