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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.
- ItemBeyond Janus Geometry: Characterization of Flow Fields around Nonspherical Photocatalytic Microswimmers(Weinheim : Wiley-VCH, 2022) Heckel, Sandra; Bilsing, Clemens; Wittmann, Martin; Gemming, Thomas; Büttner, Lars; Czarske, Jürgen; Simmchen, JulianeCatalytic microswimmers that move by a phoretic mechanism in response to a self-induced chemical gradient are often obtained by the design of spherical janus microparticles, which suffer from multi-step fabrication and low yields. Approaches that circumvent laborious multi-step fabrication include the exploitation of the possibility of nonuniform catalytic activity along the surface of irregular particle shapes, local excitation or intrinsic asymmetry. Unfortunately, the effects on the generation of motion remain poorly understood. In this work, single crystalline BiVO4 microswimmers are presented that rely on a strict inherent asymmetry of charge-carrier distribution under illumination. The origin of the asymmetrical flow pattern is elucidated because of the high spatial resolution of measured flow fields around pinned BiVO4 colloids. As a result the flow from oxidative to reductive particle sides is confirmed. Distribution of oxidation and reduction reactions suggests a dominant self-electrophoretic motion mechanism with a source quadrupole as the origin of the induced flows. It is shown that the symmetry of the flow fields is broken by self-shadowing of the particles and synthetic surface defects that impact the photocatalytic activity of the microswimmers. The results demonstrate the complexity of symmetry breaking in nonspherical microswimmers and emphasize the role of self-shadowing for photocatalytic microswimmers. The findings are leading the way toward understanding of propulsion mechanisms of phoretic colloids of various shapes.
- ItemLarge-Area Single-Crystal Graphene via Self-Organization at the Macroscale(Weinheim : Wiley-VCH, 2020) Ta, Huy Quang; Bachmatiuk, Alicja; Mendes, Rafael Gregorio; Perello, David J.; Zhao, Liang; Trzebicka, Barbara; Gemming, Thomas; Rotkin, Slava V.; Rümmeli, Mark H.In 1665 Christiaan Huygens first noticed how two pendulums, regardless of their initial state, would synchronize. It is now known that the universe is full of complex self-organizing systems, from neural networks to correlated materials. Here, graphene flakes, nucleated over a polycrystalline graphene film, synchronize during growth so as to ultimately yield a common crystal orientation at the macroscale. Strain and diffusion gradients are argued as the probable causes for the long-range cross-talk between flakes and the formation of a single-grain graphene layer. The work demonstrates that graphene synthesis can be advanced to control the nucleated crystal shape, registry, and relative alignment between graphene crystals for large area, that is, a single-crystal bilayer, and (AB-stacked) few-layer graphene can been grown at the wafer scale. © 2020 The Authors. Published by Wiley-VCH GmbH
- ItemIn 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 HermannSince 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