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  1. Article ; Online: Hydrodynamic interactions in ion transport-Theory and simulation.

    Diddens, Diddo / Heuer, Andreas

    The Journal of chemical physics

    2023  Volume 158, Issue 15

    Abstract: We present a hydrodynamic theory describing pair diffusion in systems with periodic boundary conditions, thereby generalizing earlier work on self-diffusion [B. Dünweg and K. Kremer, J. Chem. Phys. 99, 6983-6997 (1993) and I.-C. Yeh and G. Hummer, J. ... ...

    Abstract We present a hydrodynamic theory describing pair diffusion in systems with periodic boundary conditions, thereby generalizing earlier work on self-diffusion [B. Dünweg and K. Kremer, J. Chem. Phys. 99, 6983-6997 (1993) and I.-C. Yeh and G. Hummer, J. Phys. Chem. B 108, 15873-15879 (2004)]. Its predictions are compared with Molecular Dynamics simulations for a liquid carbonate electrolyte and two ionic liquids, for which we characterize the correlated motion between distinct ions. Overall, we observe good agreement between theory and simulation data, highlighting that hydrodynamic interactions universally dictate ion correlations. However, when summing over all ion pairs in the system to obtain the cross-contributions to the total cationic or anionic conductivity, the hydrodynamic interactions between ions with like and unlike charges largely cancel. Consequently, significant conductivity contributions only arise from deviations from a hydrodynamic flow field of an ideal fluid, which is from the local electrolyte structure as well as the relaxation processes in the subdiffusive regime. In the case of ionic liquids, the momentum-conservation constraint additionally is vital, which we study by employing different ionic masses in the simulations. Our formalism will likely also be helpful to estimate finite-size effects of the conductivity or of Maxwell-Stefan diffusivities in simulations.
    Language English
    Publishing date 2023-04-24
    Publishing country United States
    Document type Journal Article
    ZDB-ID 3113-6
    ISSN 1089-7690 ; 0021-9606
    ISSN (online) 1089-7690
    ISSN 0021-9606
    DOI 10.1063/5.0147339
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  2. Article ; Online: Electron transfer reaction of TEMPO-based organic radical batteries in different solvent environments: comparing quantum and classical approaches.

    Mitra, Souvik / Heuer, Andreas / Diddens, Diddo

    Physical chemistry chemical physics : PCCP

    2024  Volume 26, Issue 4, Page(s) 3020–3028

    Abstract: In this study, we delve into the complex electron transfer reactions associated with the redox-active (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO), a common component in organic radical batteries (ORBs). Our approach estimates quantum electron- ... ...

    Abstract In this study, we delve into the complex electron transfer reactions associated with the redox-active (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO), a common component in organic radical batteries (ORBs). Our approach estimates quantum electron-transfer (ET) energies using Density Functional Theory (DFT) calculations by sampling from structures simulated classically. This work presents a comparative study of reorganization energies in ET reactions across different solvents. Furthermore, we investigate how changes in the electrolyte environment can modify the reorganization energy and, consequently, impact ET dynamics. We also explore the relationship between classical and quantum vertical energies using linear regression models. Importantly, this comparison between quantum and classical vertical energies underscores the role of quantum effects, like charge delocalization, in offering added stabilization post-redox reactions. These effects are not adequately represented by the classical vertical energy distribution. Our study shows that, although we find a significant correlation between the vertical energies computed by DFT and the classical force field, the regression parameters depend on the solvent, highlighting that classical methods should be benchmarked by DFT before applying them to novel electrolyte materials.
    Language English
    Publishing date 2024-01-24
    Publishing country England
    Document type Journal Article
    ZDB-ID 1476244-4
    ISSN 1463-9084 ; 1463-9076
    ISSN (online) 1463-9084
    ISSN 1463-9076
    DOI 10.1039/d3cp04111e
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  3. Article ; Online: Study of a High-Voltage NMC Interphase in the Presence of a Thiophene Additive Realized by Operando SHINERS

    Pfeiffer, Felix / Diddens, Diddo / Weiling, Matthias / Baghernejad, Masoud

    ACS Applied Materials & Interfaces. 2023 Jan. 26, v. 15, no. 5 p.6676-6686

    2023  

    Abstract: Improving the electrochemical properties and cycle life of high-voltage cathodes in lithium-ion batteries requires a deep understanding of the structural properties and failure mechanisms at the cathode electrolyte interphase (CEI). We present a study ... ...

    Abstract Improving the electrochemical properties and cycle life of high-voltage cathodes in lithium-ion batteries requires a deep understanding of the structural properties and failure mechanisms at the cathode electrolyte interphase (CEI). We present a study implementing an advanced Raman spectroscopy technique to specifically address the compositional features of interphase during cell operation. Our operando technique, shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS), provides a reliable platform to investigate the dynamics of the interphase structure and elucidate the compositional changes near the cathode surface. To improve the CEI properties, thiophene was introduced and investigated as an effective, high-voltage film-forming additive by largely diminishing the capacity fading triggered at high potentials in LiNi₁/₃Co₁/₃Mn₁/₃O₂ cathodes. While the cells without thiophene show severe capacity fading, cells with an optimized concentration of thiophene exhibit a significant performance improvement. Operando SHINERS detects the presence of a stable CEI. The results suggest that the composition of the CEI is dominated by polythiophene and copolymerization products of ethylene carbonate with thiophene, which protects the electrolyte components from further decomposition. The formation mechanism of the polymeric film was modeled using quantum chemistry calculations, which shows good agreement with the experimental data.
    Keywords Raman spectroscopy ; carbonates ; cathodes ; copolymerization ; electrochemistry ; electrolytes ; ethylene ; interphase ; polymers ; thiophene ; lithium-ion batteries ; high-voltage cathode ; operando SHINERS
    Language English
    Dates of publication 2023-0126
    Size p. 6676-6686.
    Publishing place American Chemical Society
    Document type Article ; Online
    ISSN 1944-8252
    DOI 10.1021/acsami.2c17958
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  4. Book ; Online: Hydrodynamic Interactions in Ion Transport -- Theory and Simulation

    Diddens, Diddo / Heuer, Andreas

    2023  

    Abstract: We present a hydrodynamic theory describing pair diffusion in systems with periodic boundary conditions, thereby generalizing earlier work on self-diffusion [D\"unweg and Kremer, J. Chem. Phys. 1993, 99, 6983-6997; Yeh and Hummer, J. Phys. Chem. B 2004, ... ...

    Abstract We present a hydrodynamic theory describing pair diffusion in systems with periodic boundary conditions, thereby generalizing earlier work on self-diffusion [D\"unweg and Kremer, J. Chem. Phys. 1993, 99, 6983-6997; Yeh and Hummer, J. Phys. Chem. B 2004, 108, 15873-15879]. Its predictions are compared to Molecular Dynamics simulations for a liquid carbonate electrolyte and two ionic liquids, for which we characterize the correlated motion between distinct ions. Overall, we observe good agreement between theory and simulation data, highlighting that hydrodynamic interactions universally dictate ion correlations. However, when summing over all ion pairs in the system to obtain the cross-contributions to the total cationic or anionic conductivity, the hydrodynamic interactions between ions with like and unlike charges largely cancel. Consequently, significant conductivity contributions only arise from deviations from a hydrodynamic flow field of an ideal fluid, that is, from the local electrolyte structure as well as from relaxation processes in the subdiffusive regime. In case of ionic liquids, the momentum-conservation constraint additionally is vital, which we study by employing different ionic masses in the simulations. Our formalism will likely also be helpful to estimate finite-size effects of the conductivity or of Maxwell-Stefan diffusivities in simulations.
    Keywords Condensed Matter - Soft Condensed Matter ; Condensed Matter - Materials Science
    Subject code 541
    Publishing date 2023-02-20
    Publishing country us
    Document type Book ; Online
    Database BASE - Bielefeld Academic Search Engine (life sciences selection)

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  5. Article ; Online: Study of a High-Voltage NMC Interphase in the Presence of a Thiophene Additive Realized by Operando SHINERS.

    Pfeiffer, Felix / Diddens, Diddo / Weiling, Matthias / Baghernejad, Masoud

    ACS applied materials & interfaces

    2023  Volume 15, Issue 5, Page(s) 6676–6686

    Abstract: Improving the electrochemical properties and cycle life of high-voltage cathodes in lithium-ion batteries requires a deep understanding of the structural properties and failure mechanisms at the cathode electrolyte interphase (CEI). We present a study ... ...

    Abstract Improving the electrochemical properties and cycle life of high-voltage cathodes in lithium-ion batteries requires a deep understanding of the structural properties and failure mechanisms at the cathode electrolyte interphase (CEI). We present a study implementing an advanced Raman spectroscopy technique to specifically address the compositional features of interphase during cell operation. Our operando technique, shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS), provides a reliable platform to investigate the dynamics of the interphase structure and elucidate the compositional changes near the cathode surface. To improve the CEI properties, thiophene was introduced and investigated as an effective, high-voltage film-forming additive by largely diminishing the capacity fading triggered at high potentials in LiNi
    Language English
    Publishing date 2023-01-26
    Publishing country United States
    Document type Journal Article
    ISSN 1944-8252
    ISSN (online) 1944-8252
    DOI 10.1021/acsami.2c17958
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  6. Article ; Online: Machine Learning Isotropic

    Daniel, Davis Thomas / Mitra, Souvik / Eichel, Rüdiger-A / Diddens, Diddo / Granwehr, Josef

    Journal of chemical theory and computation

    2024  Volume 20, Issue 6, Page(s) 2592–2604

    Abstract: Methods for electronic structure computations, such as density functional theory (DFT), are routinely used for the calculation of spectroscopic parameters to establish and validate structure-parameter correlations. DFT calculations, however, are ... ...

    Abstract Methods for electronic structure computations, such as density functional theory (DFT), are routinely used for the calculation of spectroscopic parameters to establish and validate structure-parameter correlations. DFT calculations, however, are computationally expensive for large systems such as polymers. This work explores the machine learning (ML) of isotropic
    Language English
    Publishing date 2024-03-08
    Publishing country United States
    Document type Journal Article
    ISSN 1549-9626
    ISSN (online) 1549-9626
    DOI 10.1021/acs.jctc.3c01252
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  7. Article ; Online: Controlling Li

    Wettstein, Alina / Diddens, Diddo / Heuer, Andreas

    Physical chemistry chemical physics : PCCP

    2022  Volume 24, Issue 10, Page(s) 6072–6086

    Abstract: In this work, we report the results from molecular dynamics simulations of lithium salt-ionic liquid electrolytes (ILEs) based either on the symmetric bis[(trifluoromethyl)sulfonyl]imide ( ... ...

    Abstract In this work, we report the results from molecular dynamics simulations of lithium salt-ionic liquid electrolytes (ILEs) based either on the symmetric bis[(trifluoromethyl)sulfonyl]imide (TFSI
    Language English
    Publishing date 2022-03-09
    Publishing country England
    Document type Journal Article
    ZDB-ID 1476244-4
    ISSN 1463-9084 ; 1463-9076
    ISSN (online) 1463-9084
    ISSN 1463-9076
    DOI 10.1039/d1cp04830a
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  8. Article: Polymer Electrolytes in Strong External Electric Fields: Modification of Structure and Dynamics

    Wettstein, Alina / Diddens, Diddo / Heuer, Andreas

    Macromolecules. 2021 Feb. 16, v. 54, no. 5

    2021  

    Abstract: We present the results from an extensive atomistic molecular dynamics simulation study of poly(ethylene oxide) (PEO) doped with various amounts of lithium-bis(trifluoromethane)sulfonimide (LiTFSI) salt under the influence of external electric field ... ...

    Abstract We present the results from an extensive atomistic molecular dynamics simulation study of poly(ethylene oxide) (PEO) doped with various amounts of lithium-bis(trifluoromethane)sulfonimide (LiTFSI) salt under the influence of external electric field strengths up to 1 V/nm. The motivation stems from recent experimental reports on the nonlinear response of mobilities to the application of an electric field in such electrolyte systems and arising speculations on field-induced alignment of the polymer chains, creating channel-like structures that facilitate ion passage. Hence, we systematically examine the impact of electric field on the lithium coordination environment, polymer structure, as well as ionic transport properties and further present a procedure to quantify the susceptibility of both structural and dynamical observables to the external field. Our investigation reveals indeed a coiled-to-stretched transformation of the PEO strands along with a concurrent nonlinear behavior of the dynamic properties. However, from studying the temporal response of the unperturbed electrolyte system to field application, we are able to exclude a structurally conditioned enhancement of ion transport and surprisingly observe a slowing down. A microscopic understanding is achieved.
    Keywords electric field ; electrolytes ; lithium ; molecular dynamics ; motivation
    Language English
    Dates of publication 2021-0216
    Size p. 2256-2265.
    Publishing place American Chemical Society
    Document type Article
    Note NAL-AP-2-clean
    ZDB-ID 1491942-4
    ISSN 1520-5835 ; 0024-9297
    ISSN (online) 1520-5835
    ISSN 0024-9297
    DOI 10.1021/acs.macromol.0c02385
    Database NAL-Catalogue (AGRICOLA)

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  9. Article: Impact of Charged Surfaces on the Structure and Dynamics of Polymer Electrolytes: Insights from Atomistic Simulations

    Thum, Andreas / Diddens, Diddo / Heuer, Andreas

    Journal of physical chemistry. 2021 Nov. 10, v. 125, no. 46

    2021  

    Abstract: Polymer electrolytes are intensely investigated for use as solid electrolytes in next-generation lithium-ion and lithium-metal batteries. However, little is known about the structural and dynamical properties of polymer electrolytes close to electrode ... ...

    Abstract Polymer electrolytes are intensely investigated for use as solid electrolytes in next-generation lithium-ion and lithium-metal batteries. However, little is known about the structural and dynamical properties of polymer electrolytes close to electrode surfaces. Here, a PEO-Li[NTf₂] polymer electrolyte, confined between two oppositely charged graphite-like electrodes, is studied via molecular dynamics simulations. Three different surface charges of σS = 0, ±0.5 and ± 1e nm–² are considered. Upon charging, a very strong and component-specific layering is observed. Only for the highest surface charge, lithium ions get desolvated and come into direct contact with the negative electrode. The layer structure goes along with the emergence of free energy barriers, which lead to a reduction of the lithium-ion dynamics, as quantified by spatially resolved mean-square displacements, corrected for a drift component. Interchain transfers that are known to be very important for long-range lithium-ion transport in polymer electrolytes play no significant role in transitions of lithium ions between different layers.
    Keywords Gibbs free energy ; direct contact ; electrodes ; lithium ; molecular dynamics ; polymers
    Language English
    Dates of publication 2021-1110
    Size p. 25392-25403.
    Publishing place American Chemical Society
    Document type Article
    ISSN 1932-7455
    DOI 10.1021/acs.jpcc.1c07751
    Database NAL-Catalogue (AGRICOLA)

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  10. Article ; Online: Polypropylene carbonate-based electrolytes as model for a different approach towards improved ion transport properties for novel electrolytes.

    Gerlitz, Anna I / Diddens, Diddo / Grünebaum, Mariano / Heuer, Andreas / Winter, Martin / Wiemhöfer, Hans-Dieter

    Physical chemistry chemical physics : PCCP

    2023  Volume 25, Issue 6, Page(s) 4810–4823

    Abstract: Linear poly(alkylene carbonates) such as polyethylene carbonate (PEC) and polypropylene carbonate (PPC) have gained increasing interest due to their remarkable ion transport properties such as high ... ...

    Abstract Linear poly(alkylene carbonates) such as polyethylene carbonate (PEC) and polypropylene carbonate (PPC) have gained increasing interest due to their remarkable ion transport properties such as high Li
    Language English
    Publishing date 2023-02-08
    Publishing country England
    Document type Journal Article
    ZDB-ID 1476244-4
    ISSN 1463-9084 ; 1463-9076
    ISSN (online) 1463-9084
    ISSN 1463-9076
    DOI 10.1039/d2cp03756d
    Database MEDical Literature Analysis and Retrieval System OnLINE

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