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  1. AU="Thelakkat, Mukundan"
  2. AU="Morales-Ruiz, Valeria"
  3. AU=Pilotto Andrea AU=Pilotto Andrea
  4. AU="Díaz, Bogar"
  5. AU="Bennett, Christopher P"
  6. AU=Chute Christopher G.
  7. AU="Lemon, Katherine P"
  8. AU="An-Ning Zhang"
  9. AU="Ingerson-Mahar, Joseph"
  10. AU="Marie-Anne Mawhin"
  11. AU=Rizzo J Douglas
  12. AU=Anstey A

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  1. Artikel ; Online: Tuning of composition and morphology of LiFePO

    Erabhoina, Harimohan / Thelakkat, Mukundan

    Scientific reports

    2022  Band 12, Heft 1, Seite(n) 5454

    Abstract: All solid-state rechargeable lithium metal batteries (SS-LMBs) are gaining more and more importance because of their higher safety and higher energy densities in comparison to their liquid-based counterparts. In spite of this potential, their low ... ...

    Abstract All solid-state rechargeable lithium metal batteries (SS-LMBs) are gaining more and more importance because of their higher safety and higher energy densities in comparison to their liquid-based counterparts. In spite of this potential, their low discharge capacities and poor rate performances limit them to be used as state-of-the-art SS-LMBs. This arise due to the low intrinsic ionic and electronic transport pathways within the solid components in the cathode during the fast charge/discharge processes. Therefore, it is necessary to have a cathode with good electron conducting channels to increase the active material utilization without blocking the movement of lithium ions. Since SS-LMBs require a different morphology and composition of the cathode, we selected LiFePO
    Sprache Englisch
    Erscheinungsdatum 2022-03-31
    Erscheinungsland England
    Dokumenttyp Journal Article
    ZDB-ID 2615211-3
    ISSN 2045-2322 ; 2045-2322
    ISSN (online) 2045-2322
    ISSN 2045-2322
    DOI 10.1038/s41598-022-09244-3
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  2. Artikel: Solid polymer electrolytes from polyesters with diester sidechains for lithium metal batteries

    Rosenbach, Dominic / Krimalowski, Alexander / Erabhoina, Harimohan / Thelakkat, Mukundan

    Journal of materials chemistry A. 2022 Apr. 19, v. 10, no. 16

    2022  

    Abstract: A series of polymethacrylates and polyacrylates carrying diester sidechain moieties with varying alkyl spacer lengths are designed, synthesized, and evaluated as solid polymer electrolytes (SPEs) in lithium metal batteries (LMBs). These amorphous ... ...

    Abstract A series of polymethacrylates and polyacrylates carrying diester sidechain moieties with varying alkyl spacer lengths are designed, synthesized, and evaluated as solid polymer electrolytes (SPEs) in lithium metal batteries (LMBs). These amorphous polymers with glass transition temperatures in the range of −58 to +32 °C are tested as SPEs in combination with LiTFSI or LiFSI. At an optimum salt concentration of 25 wt%, ionic conductivities up to 10⁻⁴ S cm⁻¹ at 70 °C are achieved. These SPEs reveal high lithium transport numbers (0.5–0.7) and high electrochemical stability (5.4 V vs. Li/Li⁺) as determined by LSV. In combination with an ultrathin polyimide membrane and 10 wt% TiO₂ nanoparticles, dendrite-free plating/stripping at 40 and 70 °C is realized in symmetrical Li|SPE|Li cells. Detailed extended distribution of relaxation times (eDRT) analysis of impedance measurements is employed for understanding the diverse cell processes. In solvent-free LMBs comprising a polyimide membrane soaked with the nanocomposite polyester electrolyte, lithium metal foil as the anode and an optimized LiFePO₄ cathode, a very high initial specific discharge capacity of 152 mA h g⁻ ¹ (at 0.2C, 70 °C), excellent capacity retention of 94% after 100 cycles (at 1C, 70 °C) and negligible capacity fading even at 2C (96% retention after 300 cycles) are demonstrated. These novel polyester-based SPEs exhibit high cycling stability at 40 °C, making them highly attractive for room temperature applications.
    Schlagwörter ambient temperature ; anodes ; cathodes ; electrochemistry ; electrolytes ; esters ; foil ; glass transition ; lithium ; nanocomposites ; polyacrylic acid ; polyesters ; polymethylmethacrylate ; salt concentration
    Sprache Englisch
    Erscheinungsverlauf 2022-0419
    Umfang p. 8932-8947.
    Erscheinungsort The Royal Society of Chemistry
    Dokumenttyp Artikel
    ZDB-ID 2702232-8
    ISSN 2050-7496 ; 2050-7488
    ISSN (online) 2050-7496
    ISSN 2050-7488
    DOI 10.1039/d2ta00800a
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  3. Artikel ; Online: Correlating Molar Mass, π-Conjugation, and Optical Properties of Narrowly Distributed Anionic Polythiophenes in Aqueous Solutions.

    Schmidt, Martina / Karg, Matthias / Thelakkat, Mukundan / Brendel, Johannes C

    Macromolecular rapid communications

    2023  Band 45, Heft 1, Seite(n) e2300396

    Abstract: Polythiophene-based conjugated polyelectrolytes (CPE) are attracting increasing attention as sensor or interface materials in chemistry and biology. While cationic polythiophenes are better understood, limited structural information is available on their ...

    Abstract Polythiophene-based conjugated polyelectrolytes (CPE) are attracting increasing attention as sensor or interface materials in chemistry and biology. While cationic polythiophenes are better understood, limited structural information is available on their anionic counterparts. Limited access to well-defined polymers has made the study of structure-property relationships difficult and clear correlations have remained elusive. By combining controlled Kumada catalyst transfer polymerization with a polymer-analog substitution, regioregular and narrowly distributed poly(6-(thiophen-3-yl)hexane-1-sulfonate)s (PTHS) with tailored chain length are prepared. Analysis of their aqueous solution structures by small-angle neutron scattering (SANS) revealed a cylindrical conformation for all polymers tested, with a length close to the contour length of the polymer chains, while the estimated radii remain too small (<1.5 nm) for extensive π-stacking of the chains. The latter is particularly interesting as the longest polymer exhibits a concentration-independent structured absorption typical of crystalline polythiophenes. Increasing the ionic strength of the solution diminishes these features as the Coulomb repulsion between the charged repeat units is shielded, allowing the polymer to adopt a more coiled conformation. The extended π-conjugation, therefore, appears to be a key parameter for these unique optical features, which are not present in the corresponding cationic polythiophenes.
    Mesh-Begriff(e) Polymers/chemistry ; Polyelectrolytes ; Thiophenes/chemistry ; Molecular Conformation
    Chemische Substanzen polythiophene (25233-34-5) ; Polymers ; Polyelectrolytes ; Thiophenes
    Sprache Englisch
    Erscheinungsdatum 2023-08-15
    Erscheinungsland Germany
    Dokumenttyp Journal Article
    ZDB-ID 1475027-2
    ISSN 1521-3927 ; 1022-1336
    ISSN (online) 1521-3927
    ISSN 1022-1336
    DOI 10.1002/marc.202300396
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  4. Artikel ; Online: Emission modulation of fluorescent turn-on mode dibenzothienyl sulfonyl ethene photoswitches embedded in a polymer film.

    Albert, Andrea / Fried, Martina / Thelakkat, Mukundan / Köhler, Jürgen

    Physical chemistry chemical physics : PCCP

    2022  

    Abstract: For decades photochromic molecules have attracted attention for their potential in using light as an external stimulus to change their photophysical properties. Here we report the spectroscopic characterization of two emissive photochromic molecules that ...

    Abstract For decades photochromic molecules have attracted attention for their potential in using light as an external stimulus to change their photophysical properties. Here we report the spectroscopic characterization of two emissive photochromic molecules that are intrinsically fluorescent and that undergo a photocyclization/cycloreversion reaction upon illumination with light in the UV and VIS spectral ranges. For appropriately adjusted illumination intensities the emission can be modulated between the high- and the low-level with a contrast ratio exceeding 80%. The data are in reasonable agreement with the predictions from a simple kinetic model.
    Sprache Englisch
    Erscheinungsdatum 2022-12-05
    Erscheinungsland England
    Dokumenttyp Journal Article
    ZDB-ID 1476244-4
    ISSN 1463-9084 ; 1463-9076
    ISSN (online) 1463-9084
    ISSN 1463-9076
    DOI 10.1039/d2cp05062e
    Datenquelle MEDical Literature Analysis and Retrieval System OnLINE

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  5. Buch ; Online ; Dissertation / Habilitation: Polymethacrylate and Polyacrylate based Polymer and Nanocomposite Electrolytes for Lithium Metal Batteries

    Rosenbach, Dominic [Verfasser] / Thelakkat, Mukundan [Akademischer Betreuer]

    2023  

    Verfasserangabe Dominic Rosenbach ; Betreuer: Mukundan Thelakkat
    Schlagwörter Technische Chemie ; Technical Chemistry
    Thema/Rubrik (Code) sg660
    Sprache Englisch
    Verlag Universität Bayreuth
    Erscheinungsort Bayreuth
    Dokumenttyp Buch ; Online ; Dissertation / Habilitation
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  6. Artikel ; Online: Long-term switching of single photochromic triads based on dithienylcyclopentene and fluorophores at cryogenic temperatures.

    Maier, Johannes / Weller, Tina / Thelakkat, Mukundan / Köhler, Jürgen

    The Journal of chemical physics

    2021  Band 155, Heft 1, Seite(n) 14901

    Abstract: Photochromic molecules can be reversibly converted between two bistable forms by light. These systems have been intensively studied for applications as molecular memories, sensing devices, or super-resolution optical microscopy. Here, we study the long- ... ...

    Abstract Photochromic molecules can be reversibly converted between two bistable forms by light. These systems have been intensively studied for applications as molecular memories, sensing devices, or super-resolution optical microscopy. Here, we study the long-term switching behavior of single photochromic triads under oxygen-free conditions at 10 K. The triads consist of a photochromic unit that is covalently linked to two strong fluorophores that were employed for monitoring the light-induced conversions of the switch via changes in the fluorescence intensity from the fluorophores. As dyes we use either perylene bisimide or boron-dipyrromethen, and as photochromic switch we use dithienylcyclopentene (DCP). Both types of triads showed high fatigue resistance allowing for up to 6000 switching cycles of a single triad corresponding to time durations in the order of 80 min without deterioration. Long-term analysis of the switching cycles reveals that the probability that an intensity change in the emission from the dyes can be assigned to an externally stimulated conversion of the DCP (rather than to stochastic blinking of the dye molecules) amounts to 0.7 ± 0.1 for both types of triads. This number is far too low for optical data storage using single triads and implications concerning the miniaturization of optical memories based on such systems will be discussed. Yet, together with the high fatigue resistance, this number is encouraging for applications in super-resolution optical microscopy on frozen biological samples.
    Sprache Englisch
    Erscheinungsdatum 2021-07-08
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ZDB-ID 3113-6
    ISSN 1089-7690 ; 0021-9606
    ISSN (online) 1089-7690
    ISSN 0021-9606
    DOI 10.1063/5.0056815
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  7. Artikel ; Online: Highly Efficient Doping of Conjugated Polymers Using Multielectron Acceptor Salts.

    Krauss, Gert / Hochgesang, Adrian / Mohanraj, John / Thelakkat, Mukundan

    Macromolecular rapid communications

    2021  Band 42, Heft 22, Seite(n) e2100443

    Abstract: Chemical doping is a vital tool for tuning electronic properties of conjugated polymers. Most single electron acceptors used for p-doping necessitate high dopant concentrations to achieve good electrical conductivity. However, high-molar doping ratios ... ...

    Abstract Chemical doping is a vital tool for tuning electronic properties of conjugated polymers. Most single electron acceptors used for p-doping necessitate high dopant concentrations to achieve good electrical conductivity. However, high-molar doping ratios hamper doping efficiency. Here a new concept of using multielectron acceptor (MEA) salts as dopants for conjugated polymers is presented. Two novel MEA salts are synthesized and their doping efficiency towards two polymers differing in their dielectric properties are compared with two single electron acceptors such as NOPF
    Mesh-Begriff(e) Dielectric Spectroscopy ; Electric Conductivity ; Photoelectron Spectroscopy ; Polymers ; Salts
    Chemische Substanzen Polymers ; Salts
    Sprache Englisch
    Erscheinungsdatum 2021-10-22
    Erscheinungsland Germany
    Dokumenttyp Journal Article
    ZDB-ID 1475027-2
    ISSN 1521-3927 ; 1022-1336
    ISSN (online) 1521-3927
    ISSN 1022-1336
    DOI 10.1002/marc.202100443
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  8. Artikel: Sequential Co-Click Reactions with Poly(glycidyl propargyl ether) toward Single-Ion Conducting Electrolytes

    Krimalowski, Alexander / Thelakkat, Mukundan

    Macromolecules. 2019 May 30, v. 52, no. 11

    2019  

    Abstract: We utilize the direct, monomer-activated anionic ring-opening polymerization of glycidyl propargyl ether (GPE) to obtain a clickable polyether backbone [(P(GPE)] with high molecular weights and narrow distributions. First, P(GPE) was individually clicked ...

    Abstract We utilize the direct, monomer-activated anionic ring-opening polymerization of glycidyl propargyl ether (GPE) to obtain a clickable polyether backbone [(P(GPE)] with high molecular weights and narrow distributions. First, P(GPE) was individually clicked with three different azide-functionalized pendant groups: LiTFSI-N3, EG3-N3, and Bn-N3. LiTFSI serves as a lithium ion source with immobilized anion, tri(ethylene glycol) as an additional source of ion-conductive medium, and the benzyl substituent is used to improve the mechanical properties. To combine all these properties in one single polymer electrolyte, we sequentially co-clicked the named azides onto P(GPE). The final material composition, the [O]/[Li] ratio, as well as the glass transition temperature can be adjusted via the azide feed ratios. A self-standing electrolyte material with close-to-unity lithium transport number and very high electrochemical stability was obtained. We present an innovative clickable PEG platform to synthesize a ready-to-use anion-immobilized solid polymer electrolyte with tunable thermal properties in a single, sequential reaction step.
    Schlagwörter azides ; electrochemistry ; electrolytes ; glass transition temperature ; lithium ; mechanical properties ; molecular weight ; polymerization ; polymers ; thermal properties
    Sprache Englisch
    Erscheinungsverlauf 2019-0530
    Umfang p. 4042-4051.
    Erscheinungsort American Chemical Society
    Dokumenttyp Artikel
    ZDB-ID 1491942-4
    ISSN 1520-5835 ; 0024-9297
    ISSN (online) 1520-5835
    ISSN 0024-9297
    DOI 10.1021/acs.macromol.9b00206
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  9. Buch ; Online ; Dissertation / Habilitation: Polydiketopyrrolopyrroles

    Krauss, Gert [Verfasser] / Thelakkat, Mukundan [Akademischer Betreuer]

    Synthesis, Doping and Applications towards Thermoelectrics and Bioelectronics

    2022  

    Verfasserangabe Gert Krauss ; Betreuer: Mukundan Thelakkat
    Schlagwörter Naturwissenschaften ; Science
    Thema/Rubrik (Code) sg500
    Sprache Englisch
    Verlag Universität Bayreuth
    Erscheinungsort Bayreuth
    Dokumenttyp Buch ; Online ; Dissertation / Habilitation
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  10. Artikel: Elucidating the Effect of Interfacial Interactions on Crystal Orientations in Thin Films of Polythiophenes

    Dolynchuk, Oleksandr / Schmode, Philip / Fischer, Matthias / Thelakkat, Mukundan / Thurn-Albrecht, Thomas

    Macromolecules. 2021 June 03, v. 54, no. 12

    2021  

    Abstract: Molecular orientation is crucial for improving the efficiency of organic electronic devices. In many ordered materials, orientation is achieved by directional crystallization on a substrate but usually not in semicrystalline conjugated polymers. ... ...

    Abstract Molecular orientation is crucial for improving the efficiency of organic electronic devices. In many ordered materials, orientation is achieved by directional crystallization on a substrate but usually not in semicrystalline conjugated polymers. Specifically, a full face-on molecular alignment of poly(3-hexylthiophene) (P3HT) on a substrate has not been realized so far. Here, it is found that P3HT crystallized on graphene exhibits a double-layered edge-on and face-on crystal orientation with edge-on crystals formed on the top surface. This finding is interpreted as a result of two competing interfacial interactions of P3HT chains with graphene and vacuum. By modifying the side-chain chemical composition in poly[3-(6-bromohexyl)]thiophene, the influence of the interface to vacuum can be reduced, resulting in full face-on orientation in films with a thickness of up to 26 nm. These results demonstrate that directed crystallization can be used to control the orientation of semicrystalline functional polymers in thin films given that the interaction with both interfaces is taken into account.
    Schlagwörter chemical composition ; crystallization ; graphene ; thiophene
    Sprache Englisch
    Erscheinungsverlauf 2021-0603
    Umfang p. 5429-5439.
    Erscheinungsort American Chemical Society
    Dokumenttyp Artikel
    ZDB-ID 1491942-4
    ISSN 1520-5835 ; 0024-9297
    ISSN (online) 1520-5835
    ISSN 0024-9297
    DOI 10.1021/acs.macromol.0c02510
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