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  • 1.
    Bouhafs, Chamseddine
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Darakchieva, Vanya
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Persson, Ingemar
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
    Tiberj, A.
    University of Montpellier 2, France.
    Persson, Per O A
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
    Paillet, M.
    University of Montpellier 2, France.
    Zahab, A. -A.
    University of Montpellier 2, France.
    Landois, P.
    University of Montpellier 2, France.
    Juillaguet, S.
    University of Montpellier 2, France.
    Schoeche, S.
    University of Nebraska, NE 68588 USA; University of Nebraska, NE 68588 USA.
    Schubert, M.
    University of Nebraska, NE 68588 USA; University of Nebraska, NE 68588 USA.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Structural properties and dielectric function of graphene grown by high-temperature sublimation on 4H-SiC(000-1)2015In: Journal of Applied Physics, ISSN 0021-8979, E-ISSN 1089-7550, Vol. 117, no 8, p. 085701-Article in journal (Refereed)
    Abstract [en]

    Understanding and controlling growth of graphene on the carbon face (C-face) of SiC presents a significant challenge. In this work, we study the structural, vibrational, and dielectric function properties of graphene grown on the C-face of 4H-SiC by high-temperature sublimation in an argon atmosphere. The effect of growth temperature on the graphene number of layers and crystallite size is investigated and discussed in relation to graphene coverage and thickness homogeneity. An amorphous carbon layer at the interface between SiC and the graphene is identified, and its evolution with growth temperature is established. Atomic force microscopy, micro-Raman scattering spectroscopy, spectroscopic ellipsometry, and high-resolution cross-sectional transmission electron microscopy are combined to determine and correlate thickness, stacking order, dielectric function, and interface properties of graphene. The role of surface defects and growth temperature on the graphene growth mechanism and stacking is discussed, and a conclusion about the critical factors to achieve decoupled graphene layers is drawn. (C) 2015 AIP Publishing LLC.

  • 2.
    Chen, Jr-Tai
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Forsberg, Urban
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Persson, Ingemar
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
    Persson, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
    Kordina, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology. Classic WBG Semiconductors AB, LEAD, Sweden.
    Janzén, Erik
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Growth optimization of AlGaN/GaN HEMT structure on 100 mm SiC substrate: Utilizing bottom-to-top approachManuscript (preprint) (Other academic)
    Abstract [en]

    The structure of high electron mobility transistors (HEMTs) based on group-III nitride materials generally consists of three important blocks; a nucleation layer, a semi-insulating (SI) GaN buffer layer, and active layers. In this work, we present an overall growth optimization, which leads to superior crystalline quality and ultra-low thermal boundary resistance (TBR) of a 35-nm AlN nucleation layer, excellent crystalline quality of carbon-doped GaN buffer layer, and high mobility (> 2000 cm2/Vs) of two-dimensional gas (2DEG) in a simple AlGaN/GaN heterostructure grown on a SI SiC substrate.

  • 3.
    Chen, Jr-Tai
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Persson, Ingemar
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
    Nilsson, Daniel
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Hsu, Chih-Wei
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Palisaitis, Justinas
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Forsberg, Urban
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Persson, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
    Janzén, Erik
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
    Room-Temperature mobility above 2200 cm2/V.s of two-dimensional electron gas in a sharp-interface AlGaN/GaN heterostructure2015In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 106, no 25, article id 251601Article in journal (Refereed)
    Abstract [en]

    A high mobility of 2250 cm2/V·s of a two-dimensional electron gas (2DEG) in a metalorganic chemical vapor deposition-grown AlGaN/GaN heterostructure was demonstrated. The mobility enhancement was a result of better electron confinement due to a sharp AlGaN/GaN interface, as confirmed by scanning transmission electron microscopy analysis, not owing to the formation of a traditional thin AlN exclusion layer. Moreover, we found that the electron mobility in the sharp-interface heterostructures can sustain above 2000 cm2/V·s for a wide range of 2DEG densities. Finally, it is promising that the sharp-interface AlGaN/GaN heterostructure would enable low contact resistance fabrication, less impurity-related scattering, and trapping than the AlGaN/AlN/GaN heterostructure, as the high-impurity-contained AlN is removed.

  • 4.
    Halim, Joseph
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Persson, Ingemar
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Persson, Per O A
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Rosén, Johanna
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Sodium hydroxide and vacuum annealing modifications of the surface terminations of a Ti3C2 (MXene) epitaxial thin film2018In: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 8, no 64, p. 36785-36790Article in journal (Refereed)
    Abstract [en]

    We investigate, and quantify, changes in structure and surface terminations of epitaxial thin films of titanium carbide (Ti3C2) MXene, when treated by sodium hydroxide solution followed by vacuum annealing at 550 degrees C. Using X-ray photoelectron spectroscopy and scanning transmission electron microscopy, we show that NaOH treatment produce an increase in the c-lattice parameter together with an increase in the O terminations and a decrease in the F terminations. There is also an increase in the percentage of the binding energy of Ti-species in Ti 2p XPS region, which suggests an increase in the overall oxidation state of Ti. After subsequent annealing, the c-lattice parameter is slightly reduced, the overall oxidation state of Ti is decreased, and the F surface terminations are further diminished, leaving a surface with predominantly O as the surface terminating species. It is important to note that NaOH treatment facilitates removal of F at lower annealing temperatures than previously reported, which in turn is important for the range of attainable properties.

  • 5.
    Halim, Joseph
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Persson, Ingemar
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Moon, Eun Ju
    SUNY Buffalo, NY 14260 USA.
    Kuhne, Philipp
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Darakchieva, Vanya
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Persson, Per O A
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Rosén, Johanna
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Barsoum, Michel W.
    Drexel Univ, PA 19104 USA.
    Electronic and optical characterization of 2D Ti2C and Nb2C (MXene) thin films2019In: Journal of Physics: Condensed Matter, ISSN 0953-8984, E-ISSN 1361-648X, Vol. 31, no 16, article id 165301Article in journal (Refereed)
    Abstract [en]

    Two-dimensional (2D) transition metal carbides and/or nitrides (MXenes) are a new class of 2D materials, with extensive opportunities for property tailoring due to the numerous possibilities for varying chemistries and surface terminations. Here, Ti2AlC and Nb2AlC MAX phase epitaxial thin films were deposited on sapphire substrates by physical vapor deposition. The films were then etched in LiF/HCl solutions, yielding Li-intercalated, 2D Ti2CTz and Nb2CTz films, whose terminations, transport and optical properties were characterized. The former exhibits metallic conductivity, with weak localization below 50 K. In contrast, the Nb-based film exhibits an increase in resistivity with decreasing temperature from RT down to 40K consistent with variable range hopping transport. The optical properties of both films were determined from spectroscopic ellipsometry in the 0.75 to 3.50 eV range. The results for Ti2Clz films confirm the metallic behavior. In contrast, no evidence of metallic behavior is observed for the Nb2CT(z) film. The present work therefore demonstrates that one fruitful approach to alter the electronic and optical properties of MXenes is to change the nature of the transition metal.

  • 6.
    Lu, Jun
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Persson, Ingemar
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Lind, Hans
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Palisaitis, Justinas
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Li, M.
    Chinese Acad Sci, Peoples R China.
    Li, Y.
    Chinese Acad Sci, Peoples R China.
    Chen, K.
    Chinese Acad Sci, Peoples R China.
    Zhou, Jie
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Chinese Acad Sci, Peoples R China.
    Du, S.
    Chinese Acad Sci, Peoples R China.
    Chai, Z.
    Chinese Acad Sci, Peoples R China.
    Huang, Z.
    Chinese Acad Sci, Peoples R China.
    Hultman, Lars
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Rosén, Johanna
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Huang, Q.
    Chinese Acad Sci, Peoples R China.
    Persson, Per O. Å.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Tin+1Cn MXenes with fully saturated and thermally stable Cl terminations2019In: NANOSCALE ADVANCES, ISSN 2516-0230, Vol. 1, no 9, p. 3680-3685Article in journal (Refereed)
    Abstract [en]

    MXenes are a rapidly growing family of 2D materials that exhibit a highly versatile structure and composition, allowing for significant tuning of the materials properties. These properties are, however, ultimately limited by the surface terminations, which are typically a mixture of species, including F and O that are inherent to the MXene processing. Other and robust terminations are lacking. Here, we apply high-resolution scanning transmission electron microscopy (STEM), corresponding image simulations and first-principles calculations to investigate the surface terminations on MXenes synthesized from MAX phases through Lewis acidic melts. The results show that atomic Cl terminates the synthesized MXenes, with mere residual presence of other termination species. Furthermore, in situ STEM-electron energy loss spectroscopy (EELS) heating experiments show that the Cl terminations are stable up to 750 degrees C. Thus, we present an attractive new termination that widely expands the MXenes functionalization space and enables new applications.

  • 7.
    Palisaitis, Justinas
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Persson, Ingemar
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Halim, Joseph
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Rosén, Johanna
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Persson, Per O. Å.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    On the Structural Stability of MXene and the Role of Transition Metal Adatoms2018In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 10, no 23, p. 10850-10855Article in journal (Refereed)
    Abstract [en]

    In the present communication, the atomic structure and coordination of surface adsorbed species on Nb2C MXene is investigated over time. In particular, the influence of the Nb adatoms on the structural stability and oxidation behavior of the MXene is addressed. This investigation is based on plan-view geometry observations of single Nb2C MXene sheets by a combination of atomic-resolution scanning transmission electron microscopy (STEM), electron energy loss spectroscopy (EELS) and STEM image simulations.

  • 8. Order onlineBuy this publication >>
    Persson, Ingemar
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Surface characterization of 2D transition metal carbides (MXenes)2019Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Research on two-dimensional (2D) materials is a rapidly growing field owing to the wide range of new interesting properties found in 2D structures that are vastly different from their three-dimensional (3D) analogues. In addition, 2D materials embodies a significant surface area that facilitates a high degree of surface reactions per unit volume or mass, that is imperative in many applications such as catalysis, energy storage, energy conversion, filtration, and single molecule sensing. MXenes constitute a family of 2D materials consisting of transition metal carbides and/or nitrides, which are typically formed after selective etching of their 3D parent MAX phases. The latter, are a family of nanolaminated compounds that typically follow the formula Mn+1AXn (n=1-3), where M is a transition metal, A is a group 13 or 14 element, and X is C and or N. Selective etching by aqueous F- containing acids removes the A layer leaving 2D Mn+1Xn slabs instantly terminated by a mix of O-, OH- and F-groups. The first and most investigated MXene is Ti3C2TX, where TX stands for surface termination, which has shown record properties in a range of applications (eg. electrode in Li-batteries, supercapacitors, sieving membrane, electromagnetic interference shielding, and carbon capture). Adding to that, over 30 different MXenes have been discovered since 2011, exhibiting alternative or superior properties. Most importantly, elegant routes for property design in the MXene family has been demonstrated, by means of either varying the chemistry in the Mn+1Xn compound, by alloying two M elements, or by changing the structure of the MXene by introducing vacancies.

    The present work has a led to an additional route for post synthesis property tuning in MXenes by manipulation of surface termination elements. This enables a unique toolbox for property tuning which is not available to other 2D materials and is highly beneficial for applications that is dependent on surface reactions. Furthermore, chemical and structural characterization of terminations on single sheets is essential to rule out the influence of intercalants or contamination that is typically present in multilayer MXene samples or thin films. For that purpose, a method for preparing isolated contamination free single sheets of MXene samples for transmission electron microscopy (TEM) characterization was established. In order to determine vacancy and termination sites, atomically resolved scanning (S)TEM imaging and image simulations was carried out. Two main processes were employed to substitute the termination elements.

    1) An initial thermal treatment in vacuum facilitates F desorption and it was shown that O-terminations rearranges on the evacuated sites. H2 gas exposure in a controlled environment demonstrated a removal of the remaining O-terminations. As a result, termination-free MXene is possible to realize under vacuum conditions.

    2) CO2 was introduced as a first non-inherent termination on MXene by in situ CO2 gas exposure at low temperatures. That was a first demonstration of Ti3C2TX as promising material for carbon capture. Additionally, O-saturated surfaces were demonstrated after introduction of O2 gas on the F-depleted Ti3C2TX MXene, which is highly relevant for hydrogen evolution reactions where fully O-terminated Ti3C2TX are predicted to improve efficiency.

    A Lewis acid melt synthesis method was used to realize the first MXene exclusively terminated with Cl. Moreover, this was the first report of a MXene directly synthesised with terminations other than O, OH, and F.

    Furthermore, we have expanded the space of property tuning by introduction of chemical ordering, by selective etching of Y in an alloyed (Mo2/3Y1/3)2CTX MXene. This either produced chemical ordering with one M (Mo) element and vacancies, or ordering between two M (Mo and Y) elements. This was further reported to significantly increase volumetric capacitance because of the increased number of active sites around vacancies, leading to an increasing charge density. As a final note, the stability of Nb2CTX MXene under ambient conditions was investigated. It was found that the surface Nb adatoms, present after etching, got oxidized over time which resulted in local clustering and effectively degraded the MXene.

    This work has demonstrated reproducible surface characterization methods for determining termination elements and sites in 2D MXenes, that is ultimately governing MXene properties. Most importantly, we report on a new approach for MXene property tuning as well as contributing to several existing property tuning approaches. 

    List of papers
    1. On the organization and thermal behavior of functional groups on Ti3C2 MXene surfaces in vacuum
    Open this publication in new window or tab >>On the organization and thermal behavior of functional groups on Ti3C2 MXene surfaces in vacuum
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    2018 (English)In: 2D MATERIALS, ISSN 2053-1583, Vol. 5, no 1, article id 015002Article in journal (Refereed) Published
    Abstract [en]

    The two-dimensional (2D) MXene Ti(3)C(2)Tx is functionalized by surface groups (T-x) that determine its surface properties for, e.g. electrochemical applications. The coordination and thermal properties of these surface groups has, to date, not been investigated at the atomic level, despite strong variations in the MXene properties that are predicted from different coordinations and from the identity of the functional groups. To alleviate this deficiency, and to characterize the functionalized surfaces of single MXene sheets, the present investigation combines atomically resolved in situ heating in a scanning transmission electron microscope (STEM) and STEM simulations with temperature-programmed x-ray photoelectron spectroscopy (TP-XPS) in the room temperature to 750 degrees C range. Using these techniques, we follow the surface group coordination at the atomic level. It is concluded that the F and O atoms compete for the DFT-predicted thermodynamically preferred site and that at room temperature that site is mostly occupied by F. At higher temperatures, F desorbs and is replaced by O. Depending on the O/F ratio, the surface bare MXene is exposed as F desorbs, which enables a route for tailored surface functionalization.

    Place, publisher, year, edition, pages
    Institute of Physics Publishing (IOPP), 2018
    Keywords
    MXene; Ti3C2Tx in situ heating; STEM; temperature-programmed XPS; surface functionalization
    National Category
    Materials Chemistry
    Identifiers
    urn:nbn:se:liu:diva-142131 (URN)10.1088/2053-1583/aa89cd (DOI)000412302100002 ()
    Note

    Funding Agencies|Swedish Research Council [621-20124359, 622-2008-405, 2013-5580, 2016-04412, 642-2013-8020]; Knut and Alice Wallenbergs Foundation [KAW 2015.0043]; Swedish Foundation for Strategic Research (SSF) [RIF14-0074]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009 00971]

    Available from: 2017-10-24 Created: 2017-10-24 Last updated: 2019-06-28Bibliographically approved
    2. 2D Transition Metal Carbides (MXenes) for Carbon Capture
    Open this publication in new window or tab >>2D Transition Metal Carbides (MXenes) for Carbon Capture
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    2019 (English)In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 31, no 2, article id 1805472Article in journal (Refereed) Published
    Abstract [en]

    Global warming caused by burning of fossil fuels is indisputably one of mankinds greatest challenges in the 21st century. To reduce the ever-increasing CO2 emissions released into the atmosphere, dry solid adsorbents with large surface-to-volume ratio such as carbonaceous materials, zeolites, and metal-organic frameworks have emerged as promising material candidates for capturing CO2. However, challenges remain because of limited CO2/N-2 selectivity and long-term stability. The effective adsorption of CO2 gas (approximate to 12 mol kg(-1)) on individual sheets of 2D transition metal carbides (referred to as MXenes) is reported here. It is shown that exposure to N-2 gas results in no adsorption, consistent with first-principles calculations. The adsorption efficiency combined with the CO2/N-2 selectivity, together with a chemical and thermal stability, identifies the archetype Ti3C2 MXene as a new material for carbon capture (CC) applications.

    Place, publisher, year, edition, pages
    WILEY-V C H VERLAG GMBH, 2019
    Keywords
    carbon capture; environmental TEM; MXene; surface terminations
    National Category
    Materials Chemistry
    Identifiers
    urn:nbn:se:liu:diva-154119 (URN)10.1002/adma.201805472 (DOI)000455111100003 ()30393920 (PubMedID)
    Note

    Funding Agencies|Swedish Research Council [2016-04412, 2016-00889, 642-2013-8020]; Knut and Alice Wallenbergs Foundation [KAW 2015.0043]; Swedish Foundation for Strategic Research (SSF) [EM16-0004, RIF 14-0074, FL12-0181]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009 00971]

    Available from: 2019-01-29 Created: 2019-01-29 Last updated: 2019-06-28Bibliographically approved
    3. Tailoring Structure, Composition, and Energy Storage Properties of MXenes from Selective Etching of In-Plane, Chemically Ordered MAX Phases
    Open this publication in new window or tab >>Tailoring Structure, Composition, and Energy Storage Properties of MXenes from Selective Etching of In-Plane, Chemically Ordered MAX Phases
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    2018 (English)In: Small, ISSN 1613-6810, E-ISSN 1613-6829, Vol. 14, no 17, article id 1703676Article in journal (Refereed) Published
    Abstract [en]

    The exploration of 2D solids is one of our times generators of materials discoveries. A recent addition to the 2D world is MXenes that possses a rich chemistry due to the large parent family of MAX phases. Recently, a new type of atomic laminated phases (coined i-MAX) is reported, in which two different transition metal atoms are ordered in the basal planes. Herein, these i-MAX phases are used in a new route for tailoriong the MXene structure and composition. By employing different etching protocols to the parent i-MAX phase (Mo2/3Y1/3)(2)AlC, the resulting MXene can be either: i) (Mo2/3Y1/3)(2)C with in-plane elemental order through selective removal of Al atoms or ii) Mo1.33C with ordered vacancies through selective removal of both Al and Y atoms. When (Mo2/3Y1/3)(2)C (ideal stoichiometry) is used as an electrode in a supercapacitor-with KOH electrolytea volumetric capacitance exceeding 1500 F cm(-3) is obtained, which is 40% higher than that of its Mo1.33C counterpart. With H2SO4, the trend is reversed, with the latter exhibiting the higher capacitance (approximate to 1200 F cm(-3)). This additional ability for structural tailoring will indubitably prove to be a powerful tool in property-tailoring of 2D materials, as exemplified here for supercapacitors.

    Place, publisher, year, edition, pages
    WILEY-V C H VERLAG GMBH, 2018
    Keywords
    2D materials; capacitance; in-plane order; MXene; vacancies
    National Category
    Materials Chemistry
    Identifiers
    urn:nbn:se:liu:diva-147926 (URN)10.1002/smll.201703676 (DOI)000430922100010 ()29611285 (PubMedID)
    Note

    Funding Agencies|Swedish Research Council [2016-04412, 621-2012-4359, 622-2008-405, 2013-5580, 642-2013-8020, 2016-00889]; Knut and Alice Wallenbergs Foundation [KAW 2015.0043]; Swedish Foundation for Strategic Research (SSF) through the Synergy Grant FUNCASE; Swedish Foundation for Strategic Research (SSF) [RIF 14-0074]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009 00971]

    Available from: 2018-05-23 Created: 2018-05-23 Last updated: 2019-06-28
    4. On the Structural Stability of MXene and the Role of Transition Metal Adatoms
    Open this publication in new window or tab >>On the Structural Stability of MXene and the Role of Transition Metal Adatoms
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    2018 (English)In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 10, no 23, p. 10850-10855Article in journal (Refereed) Published
    Abstract [en]

    In the present communication, the atomic structure and coordination of surface adsorbed species on Nb2C MXene is investigated over time. In particular, the influence of the Nb adatoms on the structural stability and oxidation behavior of the MXene is addressed. This investigation is based on plan-view geometry observations of single Nb2C MXene sheets by a combination of atomic-resolution scanning transmission electron microscopy (STEM), electron energy loss spectroscopy (EELS) and STEM image simulations.

    Place, publisher, year, edition, pages
    Royal Society of Chemistry, 2018
    Keywords
    2D material; MXene; Scanning Transmission Electron Microscopy; Structural Stability; Adatoms
    National Category
    Chemical Sciences
    Identifiers
    urn:nbn:se:liu:diva-148143 (URN)10.1039/C8NR01986J (DOI)000435358600004 ()29870038 (PubMedID)
    Note

    Funding agencies:The authors acknowledge the Swedish Research Council for funding under grants no. 2016- 04412 and 642-2013-8020, the Knut and Alice Wallenberg’s Foundation for support of the electron microscopy laboratory in Linköping, a Fellowship grant and a project grant (KAW 2015.0043). The authors also acknowledge Swedish Foundation for Strategic Research (SSF) through the Research Infrastructure Fellow program no. RIF 14-0074. The authors finally acknowledge support from the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University (Faculty Grant SFO-Mat-LiU No 2009 00971

    Available from: 2018-05-31 Created: 2018-05-31 Last updated: 2019-06-28Bibliographically approved
  • 9.
    Persson, Ingemar
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Armakavicius, Nerijus
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Bouhafs, Chamseddine
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. Inst Italiano Tecnol, Italy.
    Stanishev, Vallery
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Kuhne, Philipp
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Hofmann, Tino
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. Univ Nebraska, NE 68588 USA; Univ Nebraska, NE 68588 USA.
    Schubert, Mathias
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. Univ Nebraska, NE 68588 USA; Univ Nebraska, NE 68588 USA.
    Rosén, Johanna
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Persson, Per O A
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Darakchieva, Vanya
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Origin of layer decoupling in ordered multilayer graphene grown by high-temperature sublimation on C-face 4H-SiC2020In: APL MATERIALS, ISSN 2166-532X, Vol. 8, no 1, article id 011104Article in journal (Refereed)
    Abstract [en]

    We study the origin of layer decoupling in ordered multilayer graphene grown by high temperature sublimation on C-face 4H-SiC. The mid-infrared optical Hall effect technique is used to determine the magnetic field dependence of the inter-Landau level transition energies and their optical polarization selection rules, which unambiguously show that the multilayer graphene consists of electronically decoupled layers. Transmission electron microscopy reveals no out-of-plane rotational disorder between layers in the stack, which is in contrast to what is typically observed for C-face graphene grown by low temperature sublimation. It is found that the multilayer graphene maintains AB-stacking order with increased interlayer spacing by 2.4%-8.4% as compared to highly oriented pyrolytic graphite. Electron energy loss spectroscopy mapping reveals Si atoms trapped in between layers, which are proposed to be the cause for the observed increased interlayer spacing leading to layer decoupling. Based on our results, we propose a defect-driven growth evolution mechanism for multilayer graphene on C-face SiC via high temperature sublimation.

  • 10.
    Persson, Ingemar
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    El Ghazaly, Ahmed
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Tao, Quanzheng
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Halim, Joseph
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Kota, Sankalp
    Drexel Univ, PA 19104 USA.
    Darakchieva, Vanya
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Palisaitis, Justinas
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Barsoum, Michel W.
    Drexel Univ, PA 19104 USA.
    Rosén, Johanna
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Persson, Per O A
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Tailoring Structure, Composition, and Energy Storage Properties of MXenes from Selective Etching of In-Plane, Chemically Ordered MAX Phases2018In: Small, ISSN 1613-6810, E-ISSN 1613-6829, Vol. 14, no 17, article id 1703676Article in journal (Refereed)
    Abstract [en]

    The exploration of 2D solids is one of our times generators of materials discoveries. A recent addition to the 2D world is MXenes that possses a rich chemistry due to the large parent family of MAX phases. Recently, a new type of atomic laminated phases (coined i-MAX) is reported, in which two different transition metal atoms are ordered in the basal planes. Herein, these i-MAX phases are used in a new route for tailoriong the MXene structure and composition. By employing different etching protocols to the parent i-MAX phase (Mo2/3Y1/3)(2)AlC, the resulting MXene can be either: i) (Mo2/3Y1/3)(2)C with in-plane elemental order through selective removal of Al atoms or ii) Mo1.33C with ordered vacancies through selective removal of both Al and Y atoms. When (Mo2/3Y1/3)(2)C (ideal stoichiometry) is used as an electrode in a supercapacitor-with KOH electrolytea volumetric capacitance exceeding 1500 F cm(-3) is obtained, which is 40% higher than that of its Mo1.33C counterpart. With H2SO4, the trend is reversed, with the latter exhibiting the higher capacitance (approximate to 1200 F cm(-3)). This additional ability for structural tailoring will indubitably prove to be a powerful tool in property-tailoring of 2D materials, as exemplified here for supercapacitors.

  • 11.
    Persson, Ingemar
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Halim, Joseph
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Hansen, Thomas W.
    DTU Danchip CEN, Denmark.
    Wagner, Jakob B.
    DTU Danchip CEN, Denmark.
    Darakchieva, Vanya
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Palisaitis, Justinas
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Rosén, Johanna
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Persson, Per O A
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    How Much Oxygen Can a MXene Surface Take Before It Breaks?2020In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, article id 1909005Article in journal (Refereed)
    Abstract [en]

    Tuning and tailoring of surface terminating functional species hold the key to unlock unprecedented properties for a wide range of applications of the largest 2D family known as MXenes. However, a few routes for surface tailoring are explored and little is known about the extent to which the terminating species can saturate the MXene surfaces. Among available terminations, atomic oxygen is of interest for electrochemical energy storage, hydrogen evolution reaction, photocatalysis, etc. However, controlled oxidation of the surfaces is not trivial due to the favored formation of oxides. In the present contribution, single sheets of Ti3C2Tx MXene, inherently terminated by F and O, are defluorinated by heating in vacuum and subsequentially exposed to O-2 gas at temperatures up to 450 degrees C in situ, in an environmental transmission electron microscope. Results include exclusive termination by O on the MXene surfaces and eventual supersaturation (x amp;gt; 2) with a retained MXene sheet structure. Upon extended O exposure, the MXene structure transforms into TiO2 and desorbs surface bound H2O and CO2 reaction products. These results are fundamental for understanding the oxidation, the presence of water on MXene surfaces, and the degradation of MXenes, and pave way for further tailoring of MXene surfaces.

  • 12.
    Persson, Ingemar
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Halim, Joseph
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Lind, Hans
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Hansen, Thomas W.
    Tech Univ Denmark DTU, Denmark.
    Wagner, Jakob B.
    Tech Univ Denmark DTU, Denmark.
    Näslund, Lars-Åke
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Darakchieva, Vanya
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Palisaitis, Justinas
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Rosén, Johanna
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Persson, Per O A
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    2D Transition Metal Carbides (MXenes) for Carbon Capture2019In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 31, no 2, article id 1805472Article in journal (Refereed)
    Abstract [en]

    Global warming caused by burning of fossil fuels is indisputably one of mankinds greatest challenges in the 21st century. To reduce the ever-increasing CO2 emissions released into the atmosphere, dry solid adsorbents with large surface-to-volume ratio such as carbonaceous materials, zeolites, and metal-organic frameworks have emerged as promising material candidates for capturing CO2. However, challenges remain because of limited CO2/N-2 selectivity and long-term stability. The effective adsorption of CO2 gas (approximate to 12 mol kg(-1)) on individual sheets of 2D transition metal carbides (referred to as MXenes) is reported here. It is shown that exposure to N-2 gas results in no adsorption, consistent with first-principles calculations. The adsorption efficiency combined with the CO2/N-2 selectivity, together with a chemical and thermal stability, identifies the archetype Ti3C2 MXene as a new material for carbon capture (CC) applications.

  • 13.
    Persson, Ingemar
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Näslund, Lars-Åke
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Halim, Joseph
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Drexel University, PA 19104 USA.
    Barsoum, Michel
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Drexel University, PA 19104 USA.
    Darakchieva, Vanya
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Palisaitis, Justinas
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Rosén, Johanna
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Persson, Per O A
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    On the organization and thermal behavior of functional groups on Ti3C2 MXene surfaces in vacuum2018In: 2D MATERIALS, ISSN 2053-1583, Vol. 5, no 1, article id 015002Article in journal (Refereed)
    Abstract [en]

    The two-dimensional (2D) MXene Ti(3)C(2)Tx is functionalized by surface groups (T-x) that determine its surface properties for, e.g. electrochemical applications. The coordination and thermal properties of these surface groups has, to date, not been investigated at the atomic level, despite strong variations in the MXene properties that are predicted from different coordinations and from the identity of the functional groups. To alleviate this deficiency, and to characterize the functionalized surfaces of single MXene sheets, the present investigation combines atomically resolved in situ heating in a scanning transmission electron microscope (STEM) and STEM simulations with temperature-programmed x-ray photoelectron spectroscopy (TP-XPS) in the room temperature to 750 degrees C range. Using these techniques, we follow the surface group coordination at the atomic level. It is concluded that the F and O atoms compete for the DFT-predicted thermodynamically preferred site and that at room temperature that site is mostly occupied by F. At higher temperatures, F desorbs and is replaced by O. Depending on the O/F ratio, the surface bare MXene is exposed as F desorbs, which enables a route for tailored surface functionalization.

1 - 13 of 13
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