Publikationen

Veröffentlichungen der Arbeitsgruppe um Prof. Dr. Andrea Balducci seit Beginn der Tätigkeit an der Friedrich-Schiller-Universität Jena

Google Scholar Profil Andrea BalducciExterner Link

81 Publikationen filtern

Die Publikationen filtern

Hervorgehobene Autoren sind Mitglieder der Forschungsgruppe.

  1. Monitoring gas evolution during ageing of industrial supercapacitors studied by in situ GC-MS

    Autoren
    M. Raidal, R. Kost, T. Makaryan, A. Balducci
    Erscheinungsjahr
    Erschienen in:
    Energy Storage Materials
    Understanding gas evolution during the ageing of electrical double layer capacitors (EDLCs) is critical for improving long-term performance and safety. However, direct gas analysis in industrial-scale cells has been hindered by their sealed design, complex internal structure, and small gas volumes, limiting broad-component analysis. This study aimed to develop and validate a novel in situ gas chromatography–mass spectrometry (GC–MS) method capable of analysing gas evolution in intact, industrial-format supercapacitor cells under realistic ageing conditions. A custom stainless-steel jig with a detachable gas extraction piece was designed to enable controlled, on-demand sampling from cylindrical EDLCs undergoing an accelerated floating ageing protocol at 3.0 V and 65°C. The system was evaluated for mechanical stability and non-intrusiveness through electrochemical performance metrics and internal pressure monitoring, while extracted gases were analysed qualitatively by GC–MS. The integrated sampling apparatus maintained normal ageing behaviour, with capacitance fading, coulombic efficiency, and logarithmic pressure growth comparable to unmodified cells. The developed in situ GC–MS technique bridges the gap between model-cell studies and real supercapacitor devices, enabling direct correlation of molecular-level gas formation with macroscopic ageing behaviour. This reliable approach provides a versatile platform for investigating alternative electrolytes, electrode materials, and ageing conditions, paving the way for deeper mechanistic understanding of supercapacitor degradation.
    Universitätsbibliographie Jena:
    fsu_mods_00029991Externer Link

  2. Method Development for Multidimensional Study of Thermal Aging in Ethyl Isopropyl Sulfone–Electrolyte Supercapacitors

    Autoren
    R. Kost, D. Leistenschneider, A. Balducci
    Erscheinungsjahr
    Erschienen in:
    Batteries and supercaps
    Understanding electrolyte degradation in electric double-layer capacitors (EDLCs) is essential for advancing high-temperature energy storage technologies. In this study, we present a comprehensive methodology to investigate temperature-induced electrolyte aging by correlating electrochemical behavior with molecular (bulk electrolyte) and interfacial (material surfaces) degradation processes. A custom-built Swagelok-type postmortem cell equipped with a quasi-reference silver wire enables simultaneous monitoring of the individual electrode potentials during operation and postaging access to both the liquid electrolyte and electrode surfaces. This integrated design allows for direct linkage between electrochemical response, liquid-phase degradation (via gas chromatography-mass spectrometry), and surface chemistry (via X-ray photoelectron spectroscopy). The methodology is validated across a matrix of electrolytes composed of the 1,1-dimethylpyrrolidinium tetrafluoroborate (Pyr ₁₁ BF ₄ ) salt in either acetonitrile (ACN), the alternative solvent ethyl isopropyl sulfone (EiPS), and an ACN:EiPS 75:25, wt% mixture. All systems were subjected to accelerated aging through 24 h voltage float tests at 3.0 V and three temperatures (20°C, 40°C, and 65°C). By selecting PYR ₁₁ BF ₄ —known for its high electrochemical and thermal stability—the degradation pathways observed can be primarily attributed to solvent effects. This work highlights the critical link between solvent decomposition and electrochemical aging, demonstrating how multidimensional postmortem analysis can guide the development of high-voltage, temperature-stable EDLCs.
    Universitätsbibliographie Jena:
    fsu_mods_00029974Externer Link

  3. Improving Electrolyte Sustainability for Sodium-Ion Capacitors by Combining a Bio-Based Solvent With a Low-Fluorine Salt

    Autoren
    A. Hainthaler, M. Pinzón, M. Arnaiz, R. Cid, Y. Lu, J. Ajuria, A. Balducci
    Erscheinungsjahr
    Erschienen in:
    ChemSusChem :: chemistry & sustainability, energy & materials
    This work focuses on improving the sustainability of electrolytes for sodium-ion capacitors (SICs). Through the combination of a low-fluorinated salt, namely sodium difluoro(oxalato)borate (NaDFOB), and the bio-based solvent γ-Valerolactone (GVL), a new electrolyte formulation (1 mol L −¹ NaDFOB in GVL) is being studied for application in SICs. Remarkably, the performance of the SIC full-cells is very comparable to the most commonly used formulation of sodium hexafluorophosphate in ethylene carbonate:propylene carbonate (1 mol L −¹ NaPF ₆ in EC:PC). Furthermore, presodiation strategies were compared for the novel electrolyte system. The in situ oxidation of a sacrificial salt (sodium squarate, Na ₂ C ₄ O ₄ ) incorporated into the positive electrode yielded comparable results to the ex situ electrochemical approach. X-ray photoelectron spectroscopy studies revealed that depending on the presodiation strategy, the solid-electrolyte-interphase composition varies significantly.
    Universitätsbibliographie Jena:
    fsu_mods_00030750Externer Link

  4. Temperature effect on hybrid capacitors containing protic acetate-based ionic liquids as electrolytes

    Autoren
    Z. Zheng, D. Leistenschneider, M. Hermesdorf, A. Balducci
    Erscheinungsjahr
    Erschienen in:
    Electrochimica acta: the journal of the International Society of Electrochemistry
    This work reports an investigation about the use of the electrolyte containing 1 M of lithium acetate (LiOAc) in the fluorine-free and low-cost protic ionic liquid 1-methylimidazolium acetate (1-MimOAc) in hybrid capacitors containing lithium iron phosphate (LFP) and activated carbon (AC) electrodes. The physicochemical properties of the electrolyte were first evaluated as a function of temperature, and its electrochemical stability window was determined by linear sweep voltammetry. We show that devices containing this electrolyte display high cycling stability, retaining 75% of their initial capacity after 4000 cycles at 25 °C. In addition, we showed that their performance is affected by the operating temperature. Specifically, at 50 °C, the activated carbon electrode undergoes oxidative surface activation and reduced stability, while at 10 °C, deposition occurs on the surface of the LFP electrode, likely associated with limited ion mobility and altered interfacial changes. These phenomena were examined by SEM, EDX and XPS analyses. These results indicate that different temperature-dependent side reactions dominate at low and high temperatures. Overall, the findings demonstrate that temperature control plays a crucial role in interfacial phase evolution and cycle performance and highlights the potential of acetate-based ionic liquids as a sustainable, fluorine-free hybrid energy storage system.
    Universitätsbibliographie Jena:
    fsu_mods_00030084Externer Link

  5. The Impact of Dual-Salt Electrolyte with Low Fluorine Content on the Performance of Layered Transition Metal Oxides for Sodium-Ion Batteries

    Autoren
    Y. Lu, M. Aslam, C. Leibing, M. Zarrabeitia, L. Roselli, L. Pfeiffer, P. Axmann, J. Geisler, P. Adelhelm, A. Balducci
    Erscheinungsjahr
    Erschienen in:
    Small : nano micro
    In this work, the characterization of novel electrolytes based on the combination of propylene carbonate (PC) solvent with sodium bis(fluorosulfonyl)imide (NaFSI) and sodium difluoro(oxalato)borate (NaDFOB), as well as their application in sodium-ion batteries (SIBs) is presented. The results show that dual-salt electrolytes have a wide electrochemical stability window, excellent transport properties, and mostly suppress anodic dissolution. When combined with P2-Na₂/₃Al₁/₉Fe₁/₉Mn₂/₃Ni₁/₉O₂(P2-AFMNO) cathode electrode for SIBs operating at 4.3 V vs Na⁺/Na, they enable high performance and stability. XPS investigation revealed that this performance is related to the formation of a thin and homogeneous cathode electrolyte interphase (CEI) at the electrode surface.
    Universitätsbibliographie Jena:
    fsu_mods_00024858Externer Link

  6. Development of Low Fluorinated, Sustainable, and Recyclable Electrolytes Based on γ-Valerolactone for High-Performance Sodium-Ion Batteries

    Autoren
    Y. Lu, M. Aslam, J. Urbano, S. Zhang, M. Zarrabeitia, T. Werner, P. Axmann, C. Leibing, A. Balducci
    Erscheinungsjahr
    Erschienen in:
    Small : nano micro
    This study introduces a dual salt novel electrolyte for sodium-ion batteries (SIBs), consisting of sodium difluoro(oxalato)borate (NaDFOB) and sodium bis(fluorosulfonyl)imide (NaFSI) salts dissolved in the bio-based γ-valerolactone (GVL) solvent. Besides its renewable origin, the electrolyte exhibited strong inhibition of anodic dissolution and excellent electrochemical stability (up to 4.3 V vs. Na ⁺ /Na). It delivered outstanding cycling stability, with ∼87 % capacity retention after 100 cycles in P2-Na ₂/₃ Al ₁/₉ Fe ₁/₉ Mn ₂/₃ Ni ₁/₉ O ₂ (P2-AFMNO) cathode half cells and ∼80 % retention after 200 cycles in lab- scale full cells with hard carbon anodes when cycled within a wide voltage window of 1.5–4.3 V. Post mortem X-ray photoelectron spectroscopy analysis helped gaining deeper understanding about the decomposition products formed on the interphases. A simple and sustainable water-based process is employed to successfully recover the GVL solvent. The recovery method enabled recover 85 % of GVL solvent from the recycling process. The feasibility of recycling is further demonstrated by reusing the recovered GVL-based electrolyte in full cells, which achieved performance comparable to that of the pristine GVL-based electrolyte and exhibited excellent long-term stability, retaining approximately 83 % of its capacity after 100 cycles.
    Universitätsbibliographie Jena:
    fsu_mods_00034461Externer Link

  7. A-Site Vacancy Engineering in KNbO₃ Perovskite for Enhanced Lithium Storage

    Autoren
    A. Khan, E. Quarez, N. Dupré, E. Gautron, A. Balducci, O. Crosnier, T. Brousse
    Erscheinungsjahr
    Erschienen in:
    Chemistry of materials : a publication of the American Chemical Society
    Universitätsbibliographie Jena:
    fsu_mods_00024160Externer Link

  8. Sodium and Potassium Storage Behaviour in AgNbO₃ Perovskite

    Autoren
    M. Orbay, A. Khan, O. Crosnier, T. Brousse, A. Balducci
    Erscheinungsjahr
    Erschienen in:
    Batteries and supercaps
    In this work, we report on the investigation the perovskite-type AgNbO₃ as a model negative electrode for sodium and potassium systems. We demonstrated that during the initial discharge, regardless of the inserted cation, the material undergoes an activation mechanism that induces a crystalline-to-amorphous transition. This transition, in turn, leads to an enhancement of the electrode capacity. At 5 A g−¹ sodium-ion AgNbO₃ and Potassium-ion AgNbO₃ display capacities of 81 mAh g−¹ and 60 mAh g−¹, respectively. Furthermore, both electrodes display good cycling stability and efficiency over 350 cycles at 1 A g−¹.
    Universitätsbibliographie Jena:
    fsu_mods_00018108Externer Link

  9. Unravelling the mechanism of potassium-ion storage into graphite through electrolyte engineering

    Autoren
    L. Meyer, A. Thiagarajan, A. Koposov, A. Balducci
    Erscheinungsjahr
    Erschienen in:
    Energy Storage Materials
    Graphite is one of the most widely used anode materials in potassium-ion batteries (PIBs). However, the exact mechanism of K⁺ions intercalation into graphite has not yet been fully understood. In addition, the intercalation process strongly depends on the selection of the electrolyte system. In this work, we evaluated the use of an electrolyte containing 1.5 M potassium bis(fluorosulfonyl)imide (KFSI) dissolved in a mixture of propylene carbonate (PC)/ 1,1,2,2-tetraethoxyethane (TEG)/ vinyl ethylene carbonate (VEC) (62:36:2 vol.%). Using such an electrolyte system it was possible to obtain experimental evidence for the formation of KC₁₆ during the potassium intercalation and deintercalation using in situ Raman spectroscopy and operando X-ray diffraction (XRD). The results are supported by the visual observation of a color change of the graphite electrode surface during the intercalation of K⁺ ions into the graphite lattice. In addition, it has been demonstrated that the selected electrolyte system eliminates the co-intercalation of the solvent into the graphite structure.
    Universitätsbibliographie Jena:
    fsu_mods_00019256Externer Link

  10. Simulations of γ-Valerolactone Solvents and Electrolytes for Lithium Batteries Using Polarizable Molecular Dynamics

    Autoren
    A. Pierini, V. Migliorati, J. Gómez-Urbano, A. Balducci, S. Brutti, E. Bodo
    Erscheinungsjahr
    Erschienen in:
    Molecules: a journal of synthetic chemistry and natural product chemistry
    In this paper, we present a molecular dynamics study of the structural and dynamical properties of γ-valerolactone (GVL) both as a standalone solvent and in electrolyte formulations for electrochemistry applications. This study involves developing a new parameterization of a polarizable forcefield and applying it to simulate pure GVL and selected salt solutions. The forcefield was validated with experimental bulk data and quantum mechanical calculations, with excellent agreement obtained in both cases. Specifically, two 1M electrolyte solutions of lithium bis(fluorosulfonyl)imide and lithium bis(oxalate)borate in GVL were simulated, focusing on their ionic transport and highlighting ion solvation structure. Ion pairing in the electrolytes was also investigated through enhanced sampling molecular dynamics, obtaining a detailed picture of the ion dynamics in the GVL solution.
    Universitätsbibliographie Jena:
    fsu_mods_00019633Externer Link

  11. Pyrrolidinium-based protic ionic liquid electrolytes for high performance RuO₂ micro-supercapacitors

    Autoren
    J. Seenath, H. Jabraoui, T. Stettner, A. Balducci, A. Estève, D. Pech, D. Rochefort
    Erscheinungsjahr
    Erschienen in:
    Electrochimica acta: the journal of the International Society of Electrochemistry
    Universitätsbibliographie Jena:
    fsu_mods_00026971Externer Link

  12. Dilithium squarate: A game-changing sacrificial salt for pre-lithiation and interphase stabilization in non-SEI forming electrolytes

    Autoren
    M. Granados-Moreno, R. Cid, M. Arnaiz, J. Gómez-Urbano, A. Balducci, E. Goikolea, J. Ajuria
    Erscheinungsjahr
    Erschienen in:
    Chemical engineering journal
    Universitätsbibliographie Jena:
    fsu_mods_00023540Externer Link
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