Tom Boenke

TU Dresden

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Stefan Kaskel

TU Dresden

Holger Althues

Fraunhofer Institute for Material and Beam Technology

Susanne Dörfler

Fraunhofer Institute for Material and Beam Technology

Thomas Abendroth

Fraunhofer Institute for Material and Beam Technology

Eike Brunner

TU Dresden

Felix Hippauf

Fraunhofer Institute for Material and Beam Technology

Konstantin Schutjajew

Friedrich Schiller University Jena

Martin Oschatz

Friedrich Schiller University Jena

Friedrich Schwotzer

TU Dresden

Paul Härtel

Fraunhofer Institute for Material and Beam Technology

Cooperative Institutions

TU Dresden

Fraunhofer Institute for Material and Beam Technology

Helmholtz-Zentrum Berlin für Materialien und Energie

Technische Universität Berlin

Robert Bosch (Germany)

Institute of Inorganic Chemistry of the Slovak Academy of Sciences

Berlin Heart (Germany)

University of Giessen

Bioanalytica (Switzerland)

Federal Institute For Materials Research and Testing

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Multimodal Operando Analysis of Lithium Sulfur Multilayer Pouch Cells: An In‐Depth Investigation on Cell Component Design and Performance

Advanced Energy Materials (2025)

Rafael Müller Tom Boenke Susanne Dörfler Thomas Abendroth Paul Härtel

Abstract This study presents an innovative operando analysis of lithium‐sulfur (Li/S) multilayer pouch cells, employing a combination of lab‐source and synchrotron x‐ray imaging to investigate sulfur crystallite dissolution and lithium dendrite formation. By integrating advanced X‐ray imaging, impedance spectroscopy, and simultaneous monitoring of temperature and pressure, the research uncovers critical insights into the behavior of active and inactive cell components. The analysis reveals significant degradation increments, primarily driven by side product accumulation and the deterioration of lithium microstructures, which contribute to performance loss over cycling. Additionally, temperature distribution analysis shows a strong correlation between joule heating, polarization resistance, and the observed endothermic processes during crystallization. These findings provide a comprehensive understanding of the mechanistic processes within industrially relevant pouch cells, highlighting opportunities for optimizing Li/S cell designs and advancing high‐energy‐density battery systems for commercial applications.

Component (thermodynamics)

Pouch

10.1002/aenm.202404256

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CCDC 2149889: Experimental Crystal Structure Determination

The Cambridge Structural Database (2022)

Sattwick Haldar Mingchao Wang Preeti Bhauriyal Arpan Hazra Arafat Hossain Khan

10.5517/ccdc.csd.cc2b548y

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Unveiling the Inner Workings of Lithium-Sulfur Pouch Cells: A Multimodal Operando Analysis Approach

Meeting abstracts/Meeting abstracts (Electrochemical Society. CD-ROM) (2023)

Rafael Müller Sebastian Risse André Hilger Nikolay Kardjilov Tom Boenke

This presentation will discuss the use of multimodal operando analysis to investigate the complex processes occurring within lithium-sulfur (Li-S) batteries during charge and discharge cycles. Li-S batteries have attracted significant attention due to their high theoretical energy density, but their practical use has been hampered by several challenges, such as poor cycling stability and low Coulombic efficiency. By using advanced techniques such as X-ray radiography, electrochemical impedance spectroscopy, force measurement, and temperature mapping, we can gain a deeper understanding of the fundamental mechanisms and degradation pathways that occur within Li-S batteries. The results describe macroscopic effects like wetting, swelling, and heating as well as microscopic phase changes, material depositions and interface properties. We will discuss how this knowledge can be used to develop improved battery materials and electrode architectures, ultimately leading to more efficient and durable Li-S batteries. Figure 1

Pouch

10.1149/ma2023-02552711mtgabs

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High-Capacity Reversible Lithium Storage in Defined Microporous Carbon Framework for All Solid-State Lithium Batteries

Luise Maria Bloi Felix Hippauf Tom Boenke Marcus Rauche Silvia Paasch

For decades graphite has been used as the anode material of choice for lithium batteries since porous carbons were believed to be inappropriate because of their high potential slope during lithiation as well as capacity losses due to intense formation of solid electrolyte interphase (SEI). However, in this work we demonstrate a microporous carbide-derived carbon material (HCmicro) to provide a high-capacity anode framework for lithium storage in all solid-state batteries. Half-cell measurements of HCmicro exhibit exceptionally high and reversible lithiation capacities of 1000 mAh g-1carbon utilizing an extremely long voltage plateau near 0 V vs. Li/Li+. The defined microporosity of the HCmicro combined well with the argyrodite-type electrolyte (Li6PS5Cl) suppressing extensive SEI formation to deliver high coulombic efficiencies. Preliminary full-cell measurements vs. NMC-cathodes (LiNi0.9Co0.05Mn0.05O2) obtained a considerably improved average potential of 3.76 V leading to a projected energy density as high as 443 Wh kg-1. 7Li Nuclear Magnetic Resonance spectroscopy was combined with ex-situ Small Angle X-ray Scattering and further electrochemical investigations to elucidate the storage mechanism of lithium inside the carbon matrix revealing the formation of extended quasi-metallic lithium clusters.

Carbon fibers

10.26434/chemrxiv.13819373

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High-Capacity Reversible Lithium Storage in Defined Microporous Carbon Framework for All Solid-State Lithium Batteries

Luise Maria Bloi Felix Hippauf Tom Boenke Marcus Rauche Silvia Paasch

For decades graphite has been used as the anode material of choice for lithium batteries since porous carbons were believed to be inappropriate because of their high potential slope during lithiation as well as capacity losses due to intense formation of solid electrolyte interphase (SEI). However, in this work we demonstrate a microporous carbide-derived carbon material (HCmicro) to provide a high-capacity anode framework for lithium storage in all solid-state batteries. Half-cell measurements of HCmicro exhibit exceptionally high and reversible lithiation capacities of 1000 mAh g -1 carbon utilizing an extremely long voltage plateau near 0 V vs. Li/Li + . The defined microporosity of the HCmicro combined well with the argyrodite-type electrolyte (Li 6 PS 5 Cl) suppressing extensive SEI formation to deliver high coulombic efficiencies. Preliminary full-cell measurements vs. NMC-cathodes (LiNi 0.9 Co 0.05 Mn 0.05 O 2 ) obtained a considerably improved average potential of 3.76 V leading to a projected energy density as high as 443 Wh kg -1 . 7 Li Nuclear Magnetic Resonance spectroscopy was combined with ex-situ Small Angle X-ray Scattering and further electrochemical investigations to elucidate the storage mechanism of lithium inside the carbon matrix revealing the formation of extended quasi-metallic lithium clusters.

Carbon fibers

10.26434/chemrxiv.13819373.v1

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Multi-Scale Analysis of Lithium-Sulfur Pouch Cells Using Imaging Methods

Meeting abstracts/Meeting abstracts (Electrochemical Society. CD-ROM) (2023)

Tobias Arlt Florian Schmidt Ralf Ziesche Sören Selve Tom Boenke

Lithium-sulfur batteries (Li-S) are promising energy storage technologies. Its high gravimetric energy density, the abundance of sulfur and low costs at high production volume, this battery type is especially applicable for automotive and aerospace applications. In recent years, the number of reported prototype cells has increased, as well as their accessible energy density. This underlines the progress of technology readiness of the Li-S system. However, despite this important breakthrough density and cycling stability have to be overcome in the Li-S research. Additionally, the influence of the cathode porosity as well as the surface of the carbon material and the electrolyte composition play an important role on the conversion of sulfur and the performance of prototype cells. Hard X-ray beamlines, as BAMline at the electron storage ring BESSY II in Berlin, Germany, have now been in service for over two decades. Several improvements have been implemented, allowing for operando tomography and fast radiographic measurements on the micrometer scale by using well-shaped synchrotron X-ray beam. In this study, operando X-ray imaging measurements on Li-S pouch cells are complemented by scanning and transmission electron microscopy and focused-ion-beam measurements on the nanometer scale delivering unique and multi-scale results about the morphology of sulfur inside the porous cathode material. Therefore, tiny pouch cells designs have been developed, allowing for operando tomography of stacked cells. Figure 1

Pouch

10.1149/ma2023-024786mtgabs

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Sulfur Transfer Melt Infiltration for High‐Power Carbon Nanotube Sheets in Lithium‐Sulfur Pouch Cells

Batteries & Supercaps (2021)

Tom Boenke Paul Härtel Susanne Dörfler Thomas Abendroth Friedrich Schwotzer

Abstract Among next‐generation battery systems, the lithium‐sulfur (Li−S) technology is attracting increasing attention driven by the low active material costs, high theoretical specific energy, and promising progress made in terms of its technology readiness level (TRL) in the recent years. However, the power density, especially in prototype cells, is an often neglected parameter being crucial for future application sectors. In this work, the cathode is redesigned by introducing a scalable, non‐toxic, and homogeneous sulfur impregnation process for free‐standing carbon scaffolds and tailorable sulfur areal loading. This novel sulfur transfer melt infiltration is exemplarily applied to process carbon nanotube (CNT)‐based Li−S cathode structures, but as a generic and scalable methodology is highly versatile. We demonstrate the development for CNT Buckypaper (BP) and CNT powder‐based dry transfer electrodes (DryFilm) as cathode host structures with the highly polysulfide (PS) solvating electrolyte system DME/DOL. In order to evaluate the practicability for high power application, the redesigned CNT BP cathode system with varying sulfur contents is employed in multi‐layered pouch cell format with 4 μL mg S −1 for reduced electrolyte conditions. Additionally, first pouch cells with circular perforated aluminum current collector enable 80 % weight savings of passive cathode material without compromising cell performance for free‐standing thin‐film cathodes. This study is an important step towards the development of lightweight Li−S cells for high power applications, such as drones or high altitude satellites.

Lithium–sulfur battery

Polysulfide

Buckypaper

10.1002/batt.202100033

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A metallic lithium anode for solid-state batteries with low volume change by utilizing a modified porous carbon host

Carbon (2024)

Stephanie Poetke Tom Boenke Kelly Henze Konstantin Schutjajew Jonas Kunigkeit

Lithium metal

Carbon fibers

10.1016/j.carbon.2024.119821

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Towards Scalable Production of Sodium‐Ion Batteries: Solvent‐Free Layered‐Oxide Cathodes and Aqueous‐Processed Hard Carbon Anodes for Cost‐Effective Full‐Cell Manufacturing.

Batteries & Supercaps (2025)

Holger Althues Joel Kuhn Florian Schmidt Pascal Seete Tom Boenke

Achieving commercial viability for more sustainable sodium‐ion batteries (SIB) necessitates reducing the environmental impact of production, particularly originating from electrode drying and the use of toxic solvents like N‐methyl‐2‐pyrrolidone (NMP). This study presents the dry‐processing of commercial P2‐type Na0.75Ni0.25Fe0.25Mn0.50O2 (NFM) via the DRYtraec® process, aiming to lower the binder content of 1 wt.% polytetrafluoroethylene (PTFE) and eliminating the need for electrode drying and NMP recovery. Assessments of electrode morphology and active material crystallinity were conducted to gauge the effects of mechanical stress during processing. The resulting cathodes, loaded at a commercially relevant 2.3‐2.7 mAh cm‐2 loading, were successfully paired with aqueous‐processed hard carbon (HC) anodes, demonstrating stable performance in full‐cells. Comparative analysis with entirely wet‐processed electrodes revealed comparable capacity accessibility and comparable long‐term stability. This showed the competitiveness of dry‐processed cathodes. Finally, the integration of NMP‐free, dry‐processed cathodes and aqueous‐processed anodes was scaled to the commercially relevant prototype pouch‐cell. The cell demonstrates stable cycling for 400 cycles with an energy density of 102 Wh kg‐1 as well as reduced processing costs and environmental footprint.

Carbon fibers

Production cost

10.1002/batt.202400572

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Mechanistic insights into the reversible lithium storage in an open porous carbon via metal cluster formation in all solid-state batteries

Carbon (2021)

Luise Maria Bloi Felix Hippauf Tom Boenke Marcus Rauche Silvia Paasch

Gravimetric analysis

Carbon fibers

10.1016/j.carbon.2021.11.061

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Citations (13)