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  1. Article: Carbon Nano-onions: Potassium Intercalation and Reductive Covalent Functionalization

    Pérez-Ojeda, M. Eugenia / Castro, Edison / Kröckel, Claudia / Lucherelli, Matteo Andrea / Ludacka, Ursula / Kotakoski, Jani / Werbach, Katharina / Peterlik, Herwig / Melle-Franco, Manuel / Chacón-Torres, Julio C. / Hauke, Frank / Echegoyen, Luis / Hirsch, Andreas / Abellán, Gonzalo

    Journal of the American Chemical Society. 2021 Oct. 26, v. 143, no. 45

    2021  

    Abstract: Herein we report the synthesis of covalently functionalized carbon nano-onions (CNOs) via a reductive approach using unprecedented alkali-metal CNO intercalation compounds. For the first time, an in situ Raman study of the controlled intercalation ... ...

    Abstract Herein we report the synthesis of covalently functionalized carbon nano-onions (CNOs) via a reductive approach using unprecedented alkali-metal CNO intercalation compounds. For the first time, an in situ Raman study of the controlled intercalation process with potassium has been carried out revealing a Fano resonance in highly doped CNOs. The intercalation was further confirmed by electron energy loss spectroscopy and X-ray diffraction. Moreover, the experimental results have been rationalized with DFT calculations. Covalently functionalized CNO derivatives were synthesized by using phenyl iodide and n-hexyl iodide as electrophiles in model nucleophilic substitution reactions. The functionalized CNOs were exhaustively characterized by statistical Raman spectroscopy, thermogravimetric analysis coupled with gas chromatography and mass spectrometry, dynamic light scattering, UV–vis, and ATR-FTIR spectroscopies. This work provides important insights into the understanding of the basic principles of reductive CNOs functionalization and will pave the way for the use of CNOs in a wide range of potential applications, such as energy storage, photovoltaics, or molecular electronics.
    Keywords Lewis acids ; Lewis bases ; Raman spectroscopy ; X-ray diffraction ; chemical bonding ; electronics ; energy ; gas chromatography ; iodides ; iodobenzenes ; mass spectrometry ; potassium ; solar energy ; thermogravimetry
    Language English
    Dates of publication 2021-1026
    Size p. 18997-19007.
    Publishing place American Chemical Society
    Document type Article
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.1c07604
    Database NAL-Catalogue (AGRICOLA)

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  2. Article: Unifying Principles of the Reductive Covalent Graphene Functionalization

    Abellán, Gonzalo / Edelthalhammer Konstantin F / Fickert Michael / Hauke Frank / Hirsch Andreas / Peterlik Herwig / Schirowski Milan / Werbach Katharina

    Journal of the American Chemical Society. 2017 Apr. 12, v. 139, no. 14

    2017  

    Abstract: Covalently functionalized graphene derivatives were synthesized via benchmark reductive routes using graphite intercalation compounds (GICs), in particular KC8. We have compared the graphene arylation and alkylation of the GIC using 4-tert- ... ...

    Abstract Covalently functionalized graphene derivatives were synthesized via benchmark reductive routes using graphite intercalation compounds (GICs), in particular KC8. We have compared the graphene arylation and alkylation of the GIC using 4-tert-butylphenyldiazonium and bis(4-(tert-butyl)phenyl)iodonium salts, as well as phenyl iodide, n-hexyl iodide, and n-dodecyl iodide, as electrophiles in model reactions. We have put a particular focus on the evaluation of the degree of addition and the bulk functionalization homogeneity (Hbulk). For this purpose, we have employed statistical Raman spectroscopy (SRS), and a forefront characterization tool using thermogravimetric analysis coupled with FT-IR, gas chromatography, and mass spectrometry (TGA/FT-IR/GC/MS). The present study unambiguously shows that the graphene functionalization using alkyl iodides leads to the best results, in terms of both the degree of addition and the Hbulk. Moreover, we have identified the reversible character of the covalent addition chemistry, even at temperatures below 200 °C. The thermally induced addend cleavage proceeds homolytically, which allows for the detection of dimeric cleavage products by TGA/FT-IR/GC/MS. This dimerization points to a certain degree of regioselectivity, leading to a low sheet homogeneity (Hsheet). Finally, we developed this concept by performing the reductive alkylation reaction in monolayer CVD graphene films. This work provides important insights into the understanding of basic principles of reductive graphene functionalization and will serve as a guide in the design of new graphene functionalization concepts.
    Keywords alkylation ; arylation ; chemical bonding ; cleavage (chemistry) ; dimerization ; Fourier transform infrared spectroscopy ; gas chromatography ; graphene ; iodides ; Lewis acids ; mass spectrometry ; models ; organoiodine compounds ; Raman spectroscopy ; regioselectivity ; temperature ; thermogravimetry
    Language English
    Dates of publication 2017-0412
    Size p. 5175-5182.
    Publishing place American Chemical Society
    Document type Article
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021%2Fjacs.7b00704
    Database NAL-Catalogue (AGRICOLA)

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  3. Article ; Online: Enhanced Thermoelectric Performance in the Ba

    Ghosh, Sanyukta / Shankar, Gyan / Karati, Anirudha / Werbach, Katharina / Rogl, Gerda / Rogl, Peter / Bauer, Ernst / Murty, B S / Suwas, Satyam / Mallik, Ramesh Chandra

    ACS applied materials & interfaces

    2020  Volume 12, Issue 43, Page(s) 48729–48740

    Abstract: The thermoelectric efficiency of skutterudite materials can be improved by lowering the lattice thermal conductivity via the uniform dispersion of a nanosized second phase in the matrix of filled ... ...

    Abstract The thermoelectric efficiency of skutterudite materials can be improved by lowering the lattice thermal conductivity via the uniform dispersion of a nanosized second phase in the matrix of filled Co
    Language English
    Publishing date 2020-10-19
    Publishing country United States
    Document type Journal Article
    ISSN 1944-8252
    ISSN (online) 1944-8252
    DOI 10.1021/acsami.0c17254
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  4. Article ; Online: Carbon Nano-onions: Potassium Intercalation and Reductive Covalent Functionalization.

    Pérez-Ojeda, M Eugenia / Castro, Edison / Kröckel, Claudia / Lucherelli, Matteo Andrea / Ludacka, Ursula / Kotakoski, Jani / Werbach, Katharina / Peterlik, Herwig / Melle-Franco, Manuel / Chacón-Torres, Julio C / Hauke, Frank / Echegoyen, Luis / Hirsch, Andreas / Abellán, Gonzalo

    Journal of the American Chemical Society

    2021  Volume 143, Issue 45, Page(s) 18997–19007

    Abstract: Herein we report the synthesis of covalently functionalized carbon nano-onions (CNOs) via a reductive approach using unprecedented alkali-metal CNO intercalation compounds. For the first time, ... ...

    Abstract Herein we report the synthesis of covalently functionalized carbon nano-onions (CNOs) via a reductive approach using unprecedented alkali-metal CNO intercalation compounds. For the first time, an
    Language English
    Publishing date 2021-10-26
    Publishing country United States
    Document type Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, Non-P.H.S.
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.1c07604
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  5. Article ; Online: Unifying Principles of the Reductive Covalent Graphene Functionalization.

    Abellán, Gonzalo / Schirowski, Milan / Edelthalhammer, Konstantin F / Fickert, Michael / Werbach, Katharina / Peterlik, Herwig / Hauke, Frank / Hirsch, Andreas

    Journal of the American Chemical Society

    2017  Volume 139, Issue 14, Page(s) 5175–5182

    Abstract: Covalently functionalized graphene derivatives were synthesized via benchmark reductive routes using graphite intercalation compounds (GICs), in particular ... ...

    Abstract Covalently functionalized graphene derivatives were synthesized via benchmark reductive routes using graphite intercalation compounds (GICs), in particular KC
    Language English
    Publishing date 2017-04-12
    Publishing country United States
    Document type Journal Article
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.7b00704
    Database MEDical Literature Analysis and Retrieval System OnLINE

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    In stock of ZB MED Bonn / Germany

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  6. Article: Exceptional Strengthening of Biodegradable Mg-Zn-Ca Alloys through High Pressure Torsion and Subsequent Heat Treatment.

    Horky, Jelena / Ghaffar, Abdul / Werbach, Katharina / Mingler, Bernhard / Pogatscher, Stefan / Schäublin, Robin / Setman, Daria / Uggowitzer, Peter J / Löffler, Jörg F / Zehetbauer, Michael J

    Materials (Basel, Switzerland)

    2019  Volume 12, Issue 15

    Abstract: In this study, two biodegradable Mg-Zn-Ca alloys with alloy content of less than 1 wt % were strengthened via high pressure torsion (HPT). A subsequent heat treatment at temperatures of around 0 ... ...

    Abstract In this study, two biodegradable Mg-Zn-Ca alloys with alloy content of less than 1 wt % were strengthened via high pressure torsion (HPT). A subsequent heat treatment at temperatures of around 0.45
    Language English
    Publishing date 2019-08-02
    Publishing country Switzerland
    Document type Journal Article
    ZDB-ID 2487261-1
    ISSN 1996-1944
    ISSN 1996-1944
    DOI 10.3390/ma12152460
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  7. Article ; Online: Phonon-tunnelling dissipation in mechanical resonators.

    Cole, Garrett D / Wilson-Rae, Ignacio / Werbach, Katharina / Vanner, Michael R / Aspelmeyer, Markus

    Nature communications

    2011  Volume 2, Page(s) 231

    Abstract: Microscale and nanoscale mechanical resonators have recently emerged as ubiquitous devices for use in advanced technological applications, for example, in mobile communications and inertial sensors, and as novel tools for fundamental scientific ... ...

    Abstract Microscale and nanoscale mechanical resonators have recently emerged as ubiquitous devices for use in advanced technological applications, for example, in mobile communications and inertial sensors, and as novel tools for fundamental scientific endeavours. Their performance is in many cases limited by the deleterious effects of mechanical damping. In this study, we report a significant advancement towards understanding and controlling support-induced losses in generic mechanical resonators. We begin by introducing an efficient numerical solver, based on the 'phonon-tunnelling' approach, capable of predicting the design-limited damping of high-quality mechanical resonators. Further, through careful device engineering, we isolate support-induced losses and perform a rigorous experimental test of the strong geometric dependence of this loss mechanism. Our results are in excellent agreement with the theory, demonstrating the predictive power of our approach. In combination with recent progress on complementary dissipation mechanisms, our phonon-tunnelling solver represents a major step towards accurate prediction of the mechanical quality factor.
    MeSH term(s) Electron Spin Resonance Spectroscopy/instrumentation ; Electron Spin Resonance Spectroscopy/methods ; Equipment Design/methods ; Equipment Failure Analysis ; Mathematical Computing ; Mechanics ; Nanotechnology/instrumentation ; Nanotechnology/methods ; Transducers
    Language English
    Publishing date 2011-03-15
    Publishing country England
    Document type Journal Article ; Research Support, Non-U.S. Gov't
    ZDB-ID 2553671-0
    ISSN 2041-1723 ; 2041-1723
    ISSN (online) 2041-1723
    ISSN 2041-1723
    DOI 10.1038/ncomms1212
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  8. Article ; Online: Exploring the Formation of Black Phosphorus Intercalation Compounds with Alkali Metals.

    Abellán, Gonzalo / Neiss, Christian / Lloret, Vicent / Wild, Stefan / Chacón-Torres, Julio C / Werbach, Katharina / Fedi, Filippo / Shiozawa, Hidetsugu / Görling, Andreas / Peterlik, Herwig / Pichler, Thomas / Hauke, Frank / Hirsch, Andreas

    Angewandte Chemie (International ed. in English)

    2017  Volume 56, Issue 48, Page(s) 15267–15273

    Abstract: Black phosphorus intercalation compounds (BPICs) with alkali metals (namely: K and Na) have been synthesized in bulk by solid-state as well as vapor-phase reactions. By means of a combination of in situ X-ray diffraction, Raman spectroscopy, and DFT ... ...

    Abstract Black phosphorus intercalation compounds (BPICs) with alkali metals (namely: K and Na) have been synthesized in bulk by solid-state as well as vapor-phase reactions. By means of a combination of in situ X-ray diffraction, Raman spectroscopy, and DFT calculations the structural behavior of the BPICs at different intercalation stages has been demonstrated for the first time. Our results provide a glimpse into the very first steps of a new family of intercalation compounds, with a distinct behavior as compared to its graphite analogues (GICs), showing a remarkable structural complexity and a dynamic behavior.
    Language English
    Publishing date 2017-10-26
    Publishing country Germany
    Document type Journal Article ; Research Support, Non-U.S. Gov't
    ZDB-ID 2011836-3
    ISSN 1521-3773 ; 1433-7851
    ISSN (online) 1521-3773
    ISSN 1433-7851
    DOI 10.1002/anie.201707462
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  9. Article ; Online: Lattice Opening upon Bulk Reductive Covalent Functionalization of Black Phosphorus.

    Wild, Stefan / Fickert, Michael / Mitrovic, Aleksandra / Lloret, Vicent / Neiss, Christian / Vidal-Moya, José Alejandro / Rivero-Crespo, Miguel Ángel / Leyva-Pérez, Antonio / Werbach, Katharina / Peterlik, Herwig / Grabau, Mathias / Wittkämper, Haiko / Papp, Christian / Steinrück, Hans-Peter / Pichler, Thomas / Görling, Andreas / Hauke, Frank / Abellán, Gonzalo / Hirsch, Andreas

    Angewandte Chemie (International ed. in English)

    2019  Volume 58, Issue 17, Page(s) 5763–5768

    Abstract: The chemical bulk reductive covalent functionalization of thin-layer black phosphorus (BP) using BP intercalation compounds has been developed. Through effective reductive activation, covalent functionalization of the charged BP by reaction with organic ... ...

    Abstract The chemical bulk reductive covalent functionalization of thin-layer black phosphorus (BP) using BP intercalation compounds has been developed. Through effective reductive activation, covalent functionalization of the charged BP by reaction with organic alkyl halides is achieved. Functionalization was extensively demonstrated by means of several spectroscopic techniques and DFT calculations; the products showed higher functionalization degrees than those obtained by neutral routes.
    Language English
    Publishing date 2019-03-21
    Publishing country Germany
    Document type Journal Article
    ZDB-ID 2011836-3
    ISSN 1521-3773 ; 1433-7851
    ISSN (online) 1521-3773
    ISSN 1433-7851
    DOI 10.1002/anie.201811181
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