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- ItemIn 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.
- ItemAdvances 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
- ItemOn 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
- ItemGraphene transfer methods: A review(New York, NY [u.a.] : Springer, 2021) Ullah, Sami; Yang, Xiaoqin; Ta, Huy Q.; Hasan, Maria; Bachmatiuk, Alicja; Tokarska, Klaudia; Trzebicka, Barbara; Fu, Lei; Rummeli, Mark H.Graphene is a material with unique properties that can be exploited in electronics, catalysis, energy, and bio-related fields. Although, for maximal utilization of this material, high-quality graphene is required at both the growth process and after transfer of the graphene film to the application-compatible substrate. Chemical vapor deposition (CVD) is an important method for growing high-quality graphene on non-technological substrates (as, metal substrates, e.g., copper foil). Thus, there are also considerable efforts toward the efficient and non-damaging transfer of quality of graphene on to technologically relevant materials and systems. In this review article, a range of graphene current transfer techniques are reviewed from the standpoint of their impact on contamination control and structural integrity preservation of the as-produced graphene. In addition, their scalability, cost- and time-effectiveness are discussed. We summarize with a perspective on the transfer challenges, alternative options and future developments toward graphene technology.
- ItemElectron Beam-Induced Reduction of Cuprite(Basel : MDPI, 2022) Siudzinska, Anna; Gorantla, Sandeep M.; Serafinczuk, Jaroslaw; Kudrawiec, Robert; Hommel, Detlef; Bachmatiuk, AlicjaCu-based materials are used in various industries, such as electronics, power generation, and catalysis. In particular, monolayered cuprous oxide (Cu2O) has potential applications in solar cells owing to its favorable electronic and magnetic properties. Atomically thin Cu2O samples derived from bulk cuprite were characterized by high-resolution transmission electron microscopy (HRTEM). Two voltages, 80 kV and 300 kV, were explored for in situ observations of the samples. The optimum electron beam parameters (300 kV, low-current beam) were used to prevent beam damage. The growth of novel crystal structures, identified as Cu, was observed in the samples exposed to isopropanol (IPA) and high temperatures. It is proposed that the exposure of the copper (I) oxide samples to IPA and temperature causes material nucleation, whereas the consequent exposure via e-beams generated from the electron beam promotes the growth of the nanosized Cu crystals.
- ItemApplications of Carbon Nanotubes in the Internet of Things Era(Berlin ; Heidelberg [u.a.] : Springer, 2021) Pang, Jinbo; Bachmatiuk, Alicja; Yang, Feng; Liu, Hong; Zhou, Weijia; Rümmeli, Mark H.; Cuniberti, GianaurelioThe post-Moore's era has boosted the progress in carbon nanotube-based transistors. Indeed, the 5G communication and cloud computing stimulate the research in applications of carbon nanotubes in electronic devices. In this perspective, we deliver the readers with the latest trends in carbon nanotube research, including high-frequency transistors, biomedical sensors and actuators, brain-machine interfaces, and flexible logic devices and energy storages. Future opportunities are given for calling on scientists and engineers into the emerging topics.
- ItemTailoring the stoichiometry of C3N4 nanosheets under electron beam irradiation(Cambridge : RSC Publ., 2021) Mendes, Rafael G.; Ta, Huy Q.; Yang, Xiaoqin; Bachmatiuk, Alicja; Praus, Petr; Mamakhel, Aref; Iversen, Bo B.; Su, Ren; Gemming, Thomas; Rümmeli, Mark H.Two-dimensional polymeric graphitic carbon nitride (g-C3N4) is a low-cost material with versatile properties that can be enhanced by the introduction of dopant atoms and by changing the degree of polymerization/stoichiometry, which offers significant benefits for numerous applications. Herein, we investigate the stability of g-C3N4 under electron beam irradiation inside a transmission electron microscope operating at different electron acceleration voltages. Our findings indicate that the degradation of g-C3N4 occurs with N species preferentially removed over C species. However, the precise nitrogen group from which N is removed from g-C3N4 (C–N–C, [double bond, length as m-dash]NH or –NH2) is unclear. Moreover, the rate of degradation increases with decreasing electron acceleration voltage, suggesting that inelastic scattering events (radiolysis) dominate over elastic events (knock-on damage). The rate of degradation by removing N atoms is also sensitive to the current density. Hence, we demonstrate that both the electron acceleration voltage and the current density are parameters with which one can use to control the stoichiometry. Moreover, as N species were preferentially removed, the d-spacing of the carbon nitride structure increased. These findings provide a deeper understanding of g-C3N4.
- ItemCrystal structure, synthesis and characterization of different chromium-based two-dimensional compounds(Riyadh : Saudi Chemical Soc., 2023) Hasan, Maria; Ta, Huy Q.; Ullah, Sami; Yang, Xiaoqin; Luo, Jingping; Bachmatiuk, Alicja; Gemming, Thomas; Trzebicka, Barbara; Mahmood, Azhar; Zeng, Mengqi; Fu, Lei; Liu, Lijun; Rümmeli, Mark H.The field of two dimensional (2D) materials experienced a surge of discoveries after the isolation of graphene. Among these, the transition metal compounds of Molybdenum and tungsten have been the most extensively studied materials after graphene. More recently, their group member chromium has only recently come to the limelight after the discovery of its exciting magnetic properties. As such the body of work surrounding 2D chromium-based materials is growing. Here, we present an up-to-date summary of the chromium 2D materials showing the latest advances in their experimental synthesis, characterization and the applications of 2D Chromium-based compounds. Finally, we conclude with a perspective on the future of 2D chromium-based materials. We believe that this study will be helpful to understand the field of chromium-based 2D compounds.
- ItemPhosphorus‐Based Composites as Anode Materials for Advanced Alkali Metal Ion Batteries(Hoboke, NJ : Wiley, 2020) Zhou, Junhua; Shi, Qitao; Ullah, Sami; Yang, Xiaoqin; Bachmatiuk, Alicja; Yang, Ruizhi; Rummeli, Mark H.Alkaline metal ion batteries, such as lithium‐ion batteries have been increasingly adopted in consumer electronics, electric vehicles, and large power grids because of their high energy density, power density and working voltage, and long cycle life. Phosphorus‐based materials including phosphorus anodes and metal phosphides with high theoretical capacity, natural abundance, and environmental friendliness show great potential as negative electrodes for alkaline metal ion batteries. In this review, based on the understanding of the storage mechanism of alkali metal ions, the scientific challenges are discussed, the preparation methods and solutions to address these challenges are summarized, the application prospects are demonstrated, and finally possible future research directions of phosphorus‐based materials are provided.
- ItemDual‐Salt Electrolyte Additives Enabled Stable Lithium Metal Anode/Lithium–Manganese‐Rich Cathode Batteries(Weinheim : Wiley-VCH, 2021) Zhou, Junhua; Lian, Xueyu; Shi, Qitao; Liu, Yu; Yang, Xiaoqin; Bachmatiuk, Alicja; Liu, Lijun; Sun, Jingyu; Yang, Ruizhi; Choi, Jin-Ho; Rummeli, Mark H.Although lithium (Li) metal anode/lithium–manganese-rich (LMR) cathode batteries have an ultrahigh energy density, the highly active Li metal and structural deterioration of LMR can make the usage of these batteries difficult. Herein, a multifunctional electrolyte containing LiBF4 and LiFSI dual-salt additives is designed, which enables the superior cyclability of Li/LMR cells with capacity retentions of ≈83.4%, 80.4%, and 76.6% after 400 cycles at 0.5, 1, and 2 C, respectively. The dual-salt electrolyte can form a thin, uniform, and inorganic species-rich solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI). In addition, it alleviates the bulk Li corrosion and enhances the structural sustainability of LMR cathode. Moreover, the electrolyte design strategy provides insights to develop other high-voltage lithium metal batteries (HVLMBs) to enhance the cycle stability.