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Now showing 1 - 10 of 10
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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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    Silicon carbide-free graphene growth on silicon for lithium-ion battery with high volumetric energy density
    (London : Nature Publishing Group, 2015) Son, In Hyuk; Park, Jong Hwan; Kwon, Soonchul; Park, Seongyong; Rümmeli, Mark H.; Bachmatiuk, Alicja; Song, Hyun Jae; Ku, Junhwan; Choi, Jang Wook; Choi, Jae-man; Doo, Seok-Gwang; Chang, Hyuk
    Silicon is receiving discernable attention as an active material for next generation lithium-ion battery anodes because of its unparalleled gravimetric capacity. However, the large volume change of silicon over charge–discharge cycles weakens its competitiveness in the volumetric energy density and cycle life. Here we report direct graphene growth over silicon nanoparticles without silicon carbide formation. The graphene layers anchored onto the silicon surface accommodate the volume expansion of silicon via a sliding process between adjacent graphene layers. When paired with a commercial lithium cobalt oxide cathode, the silicon carbide-free graphene coating allows the full cell to reach volumetric energy densities of 972 and 700 Wh l−1 at first and 200th cycle, respectively, 1.8 and 1.5 times higher than those of current commercial lithium-ion batteries. This observation suggests that two-dimensional layered structure of graphene and its silicon carbide-free integration with silicon can serve as a prototype in advancing silicon anodes to commercially viable technology.
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    Phosphorus‐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.
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    Dual‐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.
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    In Situ N-Doped Graphene and Mo Nanoribbon Formation from Mo2Ti2C3 MXene Monolayers
    (Weinheim : Wiley-VCH, 2020) Mendes, Rafael Gregorio; Ta, Huy Quang; Yang, Xiaoqin; Li, Wei; Bachmatiuk, Alicja; Choi, Jin-Ho; Gemming, Thomas; Anasori, Babak; Lijun, Liu; Fu, Lei; Liu, Zhongfan; Rümmeli, Mark Hermann
    Since the advent of monolayered 2D transition metal carbide and nitrides (MXenes) in 2011, the number of different monolayer systems and the study thereof have been on the rise. Mo2Ti2C3 is one of the least studied MXenes and new insights to this material are of value to the field. Here, the stability of Mo2Ti2C3 under electron irradiation is investigated. A transmission electron microscope (TEM) is used to study the structural and elemental changes in situ. It is found that Mo2Ti2C3 is reasonably stable for the first 2 min of irradiation. However, structural changes occur thereafter, which trigger increasingly rapid and significant rearrangement. This results in the formation of pores and two new nanomaterials, namely, N-doped graphene membranes and Mo nanoribbons. The study provides insight into the stability of Mo2Ti2C3 monolayers against electron irradiation, which will allow for reliable future study of the material using TEM. Furthermore, these findings will facilitate further research in the rapidly growing field of electron beam driven chemistry and engineering of nanomaterials. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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    CVD growth of large area smooth-edged graphene nanomesh by nanosphere lithography
    (London : Nature Publishing Group, 2013) Wang, Min; Fu, Lei; Gan, Lin; Zhang, Chaohua; Rümmeli, Mark; Bachmatiuk, Alicja; Fang, Ying; Liu, Zhongfan
    Current etching routes to process large graphene sheets into nanoscale graphene so as to open up a bandgap tend to produce structures with rough and disordered edges. This leads to detrimental electron scattering and reduces carrier mobility. In this work, we present a novel yet simple direct-growth strategy to yield graphene nanomesh (GNM) on a patterned Cu foil via nanosphere lithography. Raman spectroscopy and TEM characterizations show that the as-grown GNM has significantly smoother edges than post-growth etched GNM. More importantly, the transistors based on as-grown GNM with neck widths of 65-75 nm have a near 3-fold higher mobility than those derived from etched GNM with the similar neck widths.
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    Facile production of ultra-fine silicon nanoparticles
    (London : Royal Society Publishing, 2020) Tokarska, Klaudia; Shi, Qitao; Otulakowski, Lukasz; Wrobel, Pawel; Ta, Huy Quang; Kurtyka, Przemyslaw; Kordyka, Aleksandra; Siwy, Mariola; Vasylieva, Margaryta; Forys, Aleksander; Trzebick, Barbara; Bachmatiuk, Alicja; Rümmeli, Mark H.
    A facile procedure for the synthesis of ultra-fine silicon nanoparticles without the need for a Schlenk vacuum line is presented. The process consists of the production of a (HSiO1.5)n sol–gel precursor based on the polycondensation of low-cost trichlorosilane (HSiCl3), followed by its annealing and etching. The obtained materials were thoroughly characterized after each preparation step by electron microscopy, Fourier transform and Raman spectroscopy, X-ray dispersion spectroscopy, diffraction methods and photoluminescence spectroscopy. The data confirm the formation of ultra-fine silicon nanoparticles with controllable average diameters between 1 and 5 nm depending on the etching time.
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    Microscopic insight into the bilateral formation of carbon spirals from a symmetric iron core
    (London : Nature Publishing Group, 2013) Shiozawa, Hidetsugu; Bachmatiuk, Alicja; Stangl, Andreas; Cox, David C.; Silva, S. Ravi P.; Rümmeli, Mark; Pichler, Thomas
    Mirrored carbon-spirals have been produced from pressured ferrocene via the bilateral extrusion of the spiral pairs from an iron core. A parametric plot of the surface geometry displays the fractal growth of the conical helix made with the logarithmic spiral. Electron microscopy studies show the core is a crystalline cementite which grows and transforms its shape from spherical to biconical as it extrudes two spiralling carbon arms. In a cross section along the arms we observe graphitic flakes arranged in a herringbone structure, normal to which defects propagate. Local-wave-pattern analysis reveals nanoscale defect patterns of two-fold symmetry around the core. The data suggest that the bilateral growth originates from a globular cementite crystal with molten surfaces and the nano-defects shape emerging hexagonal carbon into a fractal structure. Understanding and knowledge obtained provide a basis for the controlled production of advanced carbon materials with designed geometries.
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    In-situ quasi-instantaneous e-beam driven catalyst-free formation of crystalline aluminum borate nanowires
    (London : Nature Publishing Group, 2016) Gonzalez-Martinez, Ignacio G.; Gemming, Thomas; Mendes, Rafael; Bachmatiuk, Alicja; Bezugly, Viktor; Kunstmann, Jens; Eckert, Jürgen; Cuniberti, Gianaurelio; Rümmeli, Mark H.
    The catalyst-assisted nucleation and growth mechanisms for many kinds of nanowires and nanotubes are pretty well understood. At times, though, 1D nanostructures form without a catalyst and the argued growth modes have inconsistencies. One such example is the catalyst-free growth of aluminium borate nanowires. Here we develop an in-situ catalyst-free room temperature growth route for aluminium nanowires using the electron beam in a transmission electron microscope. We provide strong experimental evidence that supports a formation process that can be viewed as a phase transition in which the generation of free-volume induced by the electron beam irradiation enhances the atomic mobility within the precursor material. The enhanced atomic mobility and specific features of the crystal structure of Al5BO9 drive the atomic rearrangement that results in the large scale formation of highly crystalline aluminium borate nanowires. The whole formation process can be completed within fractions of a second. Our developed growth mechanism might also be extended to describe the catalyst-free formation of other nanowires.
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    Boosting flexible electronics with integration of two-dimensional materials
    (Weinheim : Wiley, 2024) Hou, Chongyang; Zhang, Shuye; Liu, Rui; Gemming, Thomas; Bachmatiuk, Alicja; Zhao, Hongbin; Jia, Hao; Huang, Shirong; Zhou, Weijia; Xu, Jian‐Bin; Pang, Jinbo; Rümmeli, Mark H.; Bi, Jinshun; Liu, Hong; Cuniberti, Gianaurelio
    Flexible electronics has emerged as a continuously growing field of study. Two-dimensional (2D) materials often act as conductors and electrodes in electronic devices, holding significant promise in the design of high-performance, flexible electronics. Numerous studies have focused on harnessing the potential of these materials for the development of such devices. However, to date, the incorporation of 2D materials in flexible electronics has rarely been summarized or reviewed. Consequently, there is an urgent need to develop comprehensive reviews for rapid updates on this evolving landscape. This review covers progress in complex material architectures based on 2D materials, including interfaces, heterostructures, and 2D/polymer composites. Additionally, it explores flexible and wearable energy storage and conversion, display and touch technologies, and biomedical applications, together with integrated design solutions. Although the pursuit of high-performance and high-sensitivity instruments remains a primary objective, the integrated design of flexible electronics with 2D materials also warrants consideration. By combining multiple functionalities into a singular device, augmented by machine learning and algorithms, we can potentially surpass the performance of existing wearable technologies. Finally, we briefly discuss the future trajectory of this burgeoning field. This review discusses the recent advancements in flexible sensors made from 2D materials and their applications in integrated architecture and device design.