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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.
- ItemControllable sliding transfer of wafer‐size graphene(Hoboken, NJ : Wiley, 2016) Lu, Wenjing; Zeng, Mengqi; Li, Xuesong; Wang, Jiao; Tan, Lifang; Shao, Miaomiao; Han, Jiangli; Wang, Sheng; Yue, Shuanglin; Zhang, Tao; Hu, Xuebo; Mendes, Rafael G.; Rümmeli, Mark H.; Peng, Lianmao; Liu, Zhongfan; Fu, LeiThe innovative design of sliding transfer based on a liquid substrate can succinctly transfer high‐quality, wafer‐size, and contamination‐free graphene within a few seconds. Moreover, it can be extended to transfer other 2D materials. The efficient sliding transfer approach can obtain high‐quality and large‐area graphene for fundamental research and industrial applications.
- ItemIn Situ Room Temperature Electron-Beam Driven Graphene Growth from Hydrocarbon Contamination in a Transmission Electron Microscope(Basel : MDPI, 2018-5-26) Rummeli, Mark H.; Pan, Yumo; Zhao, Liang; Gao, Jing; Ta, Huy Q.; Martinez, Ignacio G.; Mendes, Rafael G.; Gemming, Thomas; Fu, Lei; Bachmatiuk, Alicja; Liu, ZhongfanThe excitement of graphene (as well as 2D materials in general) has generated numerous procedures for the fabrication of graphene. Here we present a mini-review on a rather less known, but attractive, in situ means to fabricate graphene inside a transmission electron microscope (TEM). This is achieved in a conventional TEM (viz. no sophisticated specimen holders or microscopes are required) and takes advantage of inherent hydrocarbon contamination as a carbon source. Both catalyst free and single atom catalyst approaches are reviewed. An advantage of this technique is that not only can the growth process be imaged in situ, but this can also be achieved with atomic resolution. Moreover, in the future, one can anticipate such approaches enabling the growth of nano-materials with atomic precision.
- 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.
- ItemGeneral synthesis of 2D rare-earth oxide single crystals with tailorable facets(Oxford : Oxford University Press, 2021) Li, Linyang; Lu, Fangyun; Xiong, Wenqi; Ding, Yu; Lu, Yangyi; Xiao, Yao; Tong, Xin; Wang, Yao; Jia, Shuangfeng; Wang, Jianbo; Mendes, Rafael G.; Rümmeli, Mark H.; Yuan, Shengjun; Zeng, Mengqi; Fu, LeiTwo-dimensional (2D) rare-earth oxides (REOs) are a large family of materials with various intriguing applications and precise facet control is essential for investigating new properties in the 2D limit. However, a bottleneck remains with regard to obtaining their 2D single crystals with specific facets because of the intrinsic non-layered structure and disparate thermodynamic stability of different facets. Herein, for the first time, we achieve the synthesis of a wide variety of high-quality 2D REO single crystals with tailorable facets via designing a hard-soft-acid-base couple for controlling the 2D nucleation of the predetermined facets and adjusting the growth mode and direction of crystals. Also, the facet-related magnetic properties of 2D REO single crystals were revealed. Our approach provides a foundation for further exploring other facet-dependent properties and various applications of 2D REO, as well as inspiration for the precise growth of other non-layered 2D materials.
- ItemTwinned growth behaviour of two-dimensional materials(London : Nature Publishing Group, 2016) Zhang, Tao; Jiang, Bei; Xu, Zhen; Mendes, Rafael G.; Xiao, Yao; Chen, Linfeng; Fang, Liwen; Gemming, Thomas; Chen, Shengli; Rümmeli, Mark H.; Fu, LeiTwinned growth behaviour in the rapidly emerging area of two-dimensional nanomaterials still remains unexplored although it could be exploited to fabricate heterostructure and superlattice materials. Here we demonstrate how one can utilize the twinned growth relationship between two two-dimensional materials to construct vertically stacked heterostructures. As a demonstration, we achieve 100% overlap of the two transition metal dichalcogenide layers constituting a ReS2/WS2 vertical heterostructure. Moreover, the crystal size of the stacked structure is an order of magnitude larger than previous reports. Such twinned transition metal dichalcogenides vertical heterostructures exhibit great potential for use in optical, electronic and catalytic applications. The simplicity of the twinned growth can be utilized to expand the fabrication of other heterostructures or two-dimensional material superlattice and this strategy can be considered as an enabling technology for research in the emerging field of two-dimensional van der Waals heterostructures.
- ItemIn 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
- ItemCorrection: Direct chemical vapor deposition synthesis of large area single-layer brominated grapheme (RSC Advances (2019) 9 (13527-13532) DOI: 10.1039/C9RA01152H)(London : RSC Publishing, 2019) Hasan, Maria; Meiou, Wang; Yulian, Liu; Ullah, Sami; Ta, Huy Q.; Zhao, Liang; Mendes, Rafael G.; Malik, Zahida P.; Ahmad, Nasir M.; Liu, Zhongfan; R¨ummeli, Mark H.Correction for ‘Direct chemical vapor deposition synthesis of large area single-layer brominated graphene’ by Maria Hasan et al., RSC Adv., 2019, 9, 13527–13532. In the Acknowledgements section, the attribution “the Czech Republic from ERDF “Institute of Environmental Technology – Excellent Research” (No. CZ.02.1.01/0.0/0.0/15_019/0000853), should read “the Czech Republic from ERDF OP RDE project No. CZ.02.1.01/0.0/0.0/16_019/0000853”. The Royal Society of Chemistry apologises for these errors and any consequent inconvenience to authors and readers.
- ItemDispersibility of vapor phase oxygen and nitrogen functionalized multi-walled carbon nanotubes in various organic solvents(London : Nature Publishing Group, 2016) Khazaee, Maryam; Xia, Wei; Lackner, Gerhard; Mendes, Rafael G.; Rümmeli, Mark; Muhler, Martin; Lupascu, Doru C.The synthesis and characterization of gas phase oxygen- and nitrogen-functionalized multi-walled carbon nanotubes (OMWCNTs and NMWCNTs) and the dispersibility of these tubes in organic solvents were investigated. Recently, carbon nanotubes have shown supreme capacity to effectively enhance the efficiency of organic solar cells (OSCs). A critical challenge is to individualize tubes from their bundles in order to provide homogenous nano-domains in the active layer of OSCs. OMWCNTs and NMWCNTs were synthesized via HNO3 vapor and NH3 treatments, respectively. Surface functional groups and the structure of the tubes were analyzed by temperature-programmed desorption, Fourier transform infrared spectroscopy, transmission electron microscopy, and Raman spectroscopy which confirmed the formation of functional groups on the tube surface and the enhancement of surface defects. Elemental analysis demonstrated that the oxygen and nitrogen content increased with increasing treatment time of the multi-walled carbon nanotube (MWCNT) in HNO3 vapor. According to ultra-violet visible spectroscopy, modification of the MWCNT increased the extinction coefficients of the tubes owing to enhanced compatibility of the functionalized tubes with organic matrices.
- ItemMonitoring microbial metabolites using an inductively coupled resonance circuit(London : Nature Publishing Group, 2015) Karnaushenko, Daniil; Baraban, Larysa; Ye, Dan; Uguz, Ilke; Mendes, Rafael G.; Rümmeli, Mark H.; de Visser, J. Arjan G.M.; Schmidt, Oliver G.; Cuniberti, Gianaurelio; Makarov, DenysWe present a new approach to monitor microbial population dynamics in emulsion droplets via changes in metabolite composition, using an inductively coupled LC resonance circuit. The signal measured by such resonance detector provides information on the magnetic field interaction with the bacterial culture, which is complementary to the information accessible by other detection means, based on electric field interaction, i.e. capacitive or resistive, as well as optical techniques. Several charge-related factors, including pH and ammonia concentrations, were identified as possible contributors to the characteristic of resonance detector profile. The setup enables probing the ionic byproducts of microbial metabolic activity at later stages of cell growth, where conventional optical detection methods have no discriminating power.