TY - JOUR A1 - Müller, R. A1 - Boenke, T. A1 - Dörfler, S. A1 - Abendroth, T. A1 - Härtel, P. A1 - Althues, H. A1 - Kaskel, S. A1 - Kardjilov, N. A1 - Markötter, Henning A1 - Sintschuk, Michael A1 - Hilger, A. A1 - Manke, I. A1 - Risse, S. T1 - Multimodal Operando Analysis of Lithium Sulfur Multilayer Pouch Cells: An In-Depth Investigation on Cell Component Design and Performance N2 - 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. KW - Current collector perforation KW - Impedance spectroscopy KW - Lthium sulfur batteries KW - Multilayer pouch cells KW - X-ray imaging PY - 2025 DO - https://doi.org/10.1002/aenm.202404256 SP - 1 EP - 12 PB - Wiley VHC-Verlag AN - OPUS4-62436 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Rütters, H. A1 - Fischer, S. A1 - Le, Quynh Hoa A1 - Bettge, Dirk A1 - Bäßler, Ralph A1 - Maßmann, J. A1 - Ostertag-Henning, C. A1 - Wolf, J. L. A1 - Pumpa, M. A1 - Lubenau, U. A1 - Knauer, S. A1 - Jaeger, P. A1 - Neumann, A. A1 - Svensson, K. A1 - Pöllmann, H. A1 - Lempp, C. A1 - Menezes, F. F. A1 - Hagemann, B. T1 - Towards defining reasonable minimum composition thresholds – Impacts of variable CO2 stream compositions on transport, injection and storage N2 - To set up recommendations on how to define “reasonable minimum composition thresholds” for CO2 streams to access CO2 pipeline networks, we investigated potential impacts of CO2 streams with different and temporally variable compositions and mass flow rates along the CCS chain. All investigations were based on a generic “CCS cluster scenario” in which CO2 streams captured from a spatial cluster of eleven emitters (seven fossil-fired power plants, two cement plants, one refinery and one steel mill) are collected in a regional pipeline network. The resulting CO2 stream (19.78 Mio t impure CO2 per year) is transported in a trunk line (onshore and offshore) and injected into five generic replicate storage structures (Buntsandstein saline aquifers) offshore. Experimental investigations and modeling of selected impacts revealed beneficial as well as adverse impacts of different impurities and their combinations. Overall, no fundamental technical obstacles for transporting, injecting and storing CO2 streams of the considered variable compositions and mass flow rates were observed. We recommend to define minimum composition thresholds for each specific CCS project through limiting i) the overall CO2 content, ii) maximum contents of relevant impurities or elements, iii) acceptable variability of concentrations of critical impurities, and defining impurity combinations to be avoided. KW - Impurities KW - CO2 quality KW - Pipeline network KW - Whole-chain CCS scenario KW - Recommendations PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-543004 DO - https://doi.org/10.1016/j.ijggc.2022.103589 SN - 1750-5836 VL - 114 SP - 1 EP - 14 PB - Elsevier CY - New York, NY AN - OPUS4-54300 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Heinrich, Thomas A1 - Traulsen, Christoph Hans-Henning A1 - Holzweber, Markus A1 - Richter, S. A1 - Kunz, V. A1 - Kastner, S.K. A1 - Krabbenborg, S.O. A1 - Huskens, J. A1 - Unger, Wolfgang A1 - Schalley, C.A. T1 - Coupled molecular switching processes in ordered mono- and multilayers of stimulus-responsive rotaxanes on gold surfaces N2 - Interfaces provide the structural basis for function as, for example, encountered in nature in the membrane-embedded photosystem or in technology in solar cells. Synthetic functional multilayers of molecules cooperating in a coupled manner can be fabricated on surfaces through layer-by-layer self-assembly. Ordered arrays of stimulus-responsive rotaxanes undergoing well-controlled axle shuttling are excellent candidates for coupled mechanical motion. Such stimulus-responsive surfaces may help integrate synthetic molecular machines in larger systems exhibiting even macroscopic effects or generating mechanical work from chemical energy through cooperative action. The present work demonstrates the successful deposition of ordered mono- and multilayers of chemically switchable rotaxanes on gold surfaces. Rotaxane mono- and multilayers are shown to reversibly switch in a coupled manner between two ordered states as revealed by linear dichroism effects in angle-resolved NEXAFS spectra. Such a concerted switching process is observed only when the surfaces are well packed, while less densely packed surfaces lacking lateral order do not exhibit such effects. KW - Molecular machine KW - Rotaxane KW - LBL growth KW - XPS KW - NEXAFS KW - SIMS PY - 2015 DO - https://doi.org/10.1021/ja512654d SN - 0002-7863 SN - 1520-5126 VL - 137 IS - 13 SP - 4382 EP - 4390 PB - American Chemical Society CY - Washington, DC, USA AN - OPUS4-33077 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Sun, F. A1 - Wang, C. A1 - Osenberg, M. A1 - Dong, K. A1 - Zhang, S. A1 - Yang, C. A1 - Wang, Y. A1 - Hilger, A. A1 - Zhang, J. A1 - Dong, S. A1 - Markötter, Henning A1 - Manke, I. A1 - Cui, G. T1 - Clarifying the Electro-Chemo-Mechanical Coupling in Li10SnP2S12 based All-Solid-State Batteries N2 - A fundamental clarification of the electro-chemo-mechanical coupling at the solid–solid electrode|electrolyte interface in all-solid-state batteries (ASSBs) is of crucial significance but has proven challenging. Herein, (synchrotron) X-ray tomography, electrochemical impedance spectroscopy (EIS), time-of-flight secondary-ion mass spectrometry (TOF-SIMS), and finite element analysis (FEA) modeling are jointly used to decouple the electro-chemo-mechanical coupling in Li10SnP2S12-based ASSBs. Non-destructive (synchrotron) X-ray tomography results visually disclose unexpected mechanical deformation of the solid electrolyte and electrode as well as an unanticipated evolving behavior of the (electro)chemically generated interphase. The EIS and TOFSIMS probing results provide additional information that links the interphase/electrode properties to the overall battery performance. The modeling results complete the picture by providing the detailed distribution of the mechanical stress/strain and the potential/ionic flux within the electrolyte. Collectively, these results suggest that 1) the interfacial volume changes induced by the (electro)chemical reactions can trigger the mechanical deformation of the solid electrode and electrolyte; 2) the overall electrochemical process can accelerate the interfacial chemical reactions; 3) the reconfigured interfaces in turn influence the electric potential distribution as well as charge transportation within the SE. These fundamental discoveries that remain unreported until now significantly improve the understanding of the complicated electro-chemo-mechanical couplings in ASSBs. KW - All-solid-state batteries KW - Lithium metal batteries KW - Solid electrolytes KW - Sulfide solid electrolytes KW - Synchrotron X-ray tomography PY - 2022 DO - https://doi.org/10.1002/aenm.202103714 SN - 1614-6832 SP - 2103714 PB - Wiley VHC-Verlag AN - OPUS4-54431 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Göbel, M. A1 - Kirsch, S. A1 - Schwarze, L: A1 - Schmidt, L. A1 - Scholz, H. A1 - Haußmann, J. A1 - Klages, M. A1 - Scholta, J. A1 - Markötter, Henning A1 - Alrwashdeh, S. A1 - Manke, I. A1 - Müller, Bernd R. T1 - Transient limiting current measurements for characterization of gas diffusion layers N2 - The water management in proton exchange membrane fuel cells (PEMFC) is strongly influenced by the design of the gas diffusion layers (GDL). Limiting current measurements in small-scale cells operating at high stoichiometries are useful to determine the oxygen transport resistance. The oxygen transport resistance increases, once water condenses inside the GDL. In this study a new electrochemical method for voltage loss estimation of GDL induced oxygen transport losses are presented. This new method, referred to as “transient limiting current” (TLC), is compared with the literature method. TLC allows a direct estimation of oxygen transport resistance at an arbitrarily conditioned state. This study also presents a case study of liquid water visualization of a PEM fuel cell with varying GDLs types. With the help of quasi in-situ synchrotron X-ray computed tomography and time resolved radiography measurements we investigate appearance and distribution of liquid water inside the GDLs under limiting current conditions. KW - In-situ characterization of GDLs KW - In-situ synchrotron X-ray computed tomography KW - In-situ synchrotron X-ray radiography KW - BAMline PY - 2018 DO - https://doi.org/10.1016/j.jpowsour.2018.09.003 SN - 0378-7753 SN - 1873-2755 VL - 402 SP - 237 EP - 245 PB - Elsevier B.V. AN - OPUS4-46552 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Alrwashdeh, S. S. A1 - Markötter, Henning A1 - Haußmann, J. A1 - Hilger, A. A1 - Klages, M. A1 - Müller, Bernd R. A1 - Kupsch, Andreas A1 - Riesemeier, Heinrich A1 - Scholta, J. A1 - Manke, I. T1 - Investigation of water transport in newly developed micro porous layers for polymer electrolyte membrane fuel cells N2 - In this investigation, synchrotron X-ray imaging was used to investigate the water distribution inside newly developed gas diffusion media in polymer electrolyte membrane fuel cells. In-situ radiography was used to reveal the relationship between the structure of the microporous layer (MPL) and the water flow in a newly developed MPL equipped with randomly arranged holes. A strong influence of these holes on the overall water transport was found. This contribution provides a brief overview to some of our recent activities on this research field. KW - Polymer electrolyte membrane fuel cell KW - Microporous layer KW - Water distribution KW - Radiography KW - Synchrotron X-ray imaging PY - 2017 DO - https://doi.org/10.9729/AM.2017.47.3.101 SN - 2287-4445 SN - 2287-5123 VL - 47 IS - 3 SP - 101 EP - 104 AN - OPUS4-43356 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Risse, S. A1 - Juhl, A. A1 - Mascotto, S. A1 - Arlt, T. A1 - Markötter, Henning A1 - Hilger, A. A1 - Manke, I. A1 - Fröba, M. T1 - Detailed and Direct Observation of Sulfur Crystal Evolution During Operando Analysis of a Li-S Cell with Synchrotron Imaging N2 - Herein, we present a detailed investigation of the electrochemically triggered formation and dissolution processes of α- and β-sulfur crystals on a monolithic carbon cathode using operando high-resolution synchrotron radiography (438 nm/pixel). The combination of visual monitoring with the electrical current response during cyclic voltammetry provides valuable insights into the sulfur formation and dissolution mechanism. Our observations show that the crystal growth process is mainly dictated by a rapid equilibrium between long-chain polysulfides on one side and solid sulfur/short-chain polysulfides on the other side, which is consistent with previous studies in this field. The high temporal and spatial resolution of synchrotron imaging enables the observation of different regimes during the sulfur formation and dissolution process. The appearance of short-chain polysulfides after the first anodic CV peak initiates a rapid dissolution process of α-sulfur crystals on the cathode. The increase in the long-chain lithium polysulfide concentration at the cathode surface during charge results in an increased crystal growth rate, which in turn produces imperfections in α- and β-sulfur crystals. There are strong indications that these defects are fluid inclusions, which may trap dissolved polysulfides and therefore reduce the electrochemical cell capacity. KW - LiS battery KW - Radiography KW - Synchrotron Imaging PY - 2020 DO - https://doi.org/10.1021/acs.jpclett.0c01284 VL - 11 IS - 14 SP - 5674 EP - 5679 AN - OPUS4-51100 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Tran, K. V. A1 - Woracek, R. A1 - Kardjilov, N. A1 - Markötter, Henning A1 - Hilger, A. A1 - Kockelmann, W. A1 - Kelleher, J. A1 - Puplampu, S. B. A1 - Penumadu, D. A1 - Tremsin, A. S. A1 - Banhart, J. A1 - Manke, I. T1 - Spectral neutron tomography N2 - Combined three-dimensional (3D) mapping of (micro-)structures with elemental and crystalline phase variations is of significant importance for the characterization of materials. Neutron wavelength selective imaging is a spectral imaging technique that exploits unique contrast differences e.g. for mapping dissimilar elemental, isotope, or phase compositions, and has the particular advantage of being applicable to sample volumes on the meso- and macroscale. While being mostly applied as radiography (2D) so far, we herein report that the extension to tomography allows for the display of the full spectral information for every voxel and in 3D. The development is supported by example data from a continuous as well as a pulsed neutron source. As a practical example, we collected 4D data sets (3D + spectral) of plastically deformed metastable stainless steel and herein demonstrate an improved quantification strategy for crystalline phase fractions. These exemplary results illustrate that localized phase transformations can be quantified even in complex geometries within centimeter-sized samples, and we will discuss the limits and future prospects of the technique that is not limited to crystalline materials. KW - 4D tomographic data KW - Multi-energy CT KW - Spectral CT KW - Phase distribution KW - Full-field phase tomography PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-521668 DO - https://doi.org/10.1016/j.mtadv.2021.100132 VL - 9 SP - 132 PB - Elsevier Ltd. AN - OPUS4-52166 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Zhang, X. A1 - Zhang, S. A1 - Lu, J. A1 - Tang, F. A1 - Dong, K. A1 - Yu, Z. A1 - Hilger, A. A1 - Osenberg, M. A1 - Markötter, Henning A1 - Wilde, F. A1 - Zhang, S. A1 - Zhao, J. A1 - Xu, G. A1 - Manke, I. A1 - Sun, F. A1 - Cui, G. T1 - Unveiling the Electro-Chemo-Mechanical Failure Mechanism of Sodium Metal Anodes in Sodium–Oxygen Batteries by Synchrotron X-Ray Computed Tomography N2 - Rechargeable sodium–oxygen batteries (NaOBs) are receiving extensive research interests because of their advantages such as ultrahigh energy density and cost efficiency. However, the severe failure of Na metal anodes has impeded the commercial development of NaOBs. Herein, combining in situ synchrotron X-ray computed tomography (SXCT) and other complementary characterizations, a novel electro-chemo-mechanical failure mechanism of sodium metal anode in NaOBs is elucidated. It is visually showcased that the Na metal anodes involve a three-stage decay evolution of a porous Na reactive interphase layer (NRIL): from the initially dot-shaped voids evolved into the spindle-shaped voids and the eventually-developed ruptured cracks. The initiation of this three-stage evolution begins with chemical-resting and is exacerbated by further electrochemical cycling. From corrosion science and fracture mechanics, theoretical simulations suggest that the evolution of porous NRIL is driven by the concentrated stress at crack tips. The findings illustrate the importance of preventing electro-chemo-mechanical degradation of Na anodes in practically rechargeable NaOBs. KW - Synchrotron radiation KW - X-ray imaging KW - NaO-battery PY - 2024 DO - https://doi.org/10.1002/adfm.202402253 SN - 1616-301X SP - 1 EP - 12 PB - Wiley VHC-Verlag AN - OPUS4-59820 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Rütters, H. A1 - Fischer, S. A1 - Le, Quynh A1 - Bettge, Dirk A1 - Bäßler, Ralph A1 - Maßmann, J. A1 - Ostertag-Henning, C. A1 - Wolf, J. Lennard A1 - Pumpa, M. A1 - Lubenau, U. A1 - Knauer, S. A1 - Jaeger, P. A1 - Neumann, A. A1 - Svensson, K. A1 - Lempp, C. A1 - Menezes, F. A1 - Hagemann, B. T1 - Towards defining reasonable minimum composition thresholds – impacts of variable CO2 stream compositions on transport, injection and storage N2 - The collaborative project “Impacts of impurities in CO2 streams captured from different emitters in a regional cluster on transport, injection and storage (CLUSTER)” aimed to set up recommendations on how to define “reasonable minimum composition thresholds” that CO2 streams should meet when accessing CO2 transport pipeline networks. Within CLUSTER, we investigated potential impacts of CO2 streams with different and temporally variable compositions and mass flow rates along the whole CCS chain. Investigations included, amongst others, impacts on: Corrosion of pipeline steel, pipeline network design and related transport costs, alteration of well bore cements, pressure development and rock integrity, geochemical reactions, and petrophysical and geomechanical rock properties. All investigations are based on a generic CCS chain scenario. In this scenario, CO2 streams are captured from a spatial cluster of eleven emitters and collected in a regional pipeline network. Emitters comprise seven fossil fuel-fired power plants equipped with different capture technologies, two cement plants, one refinery and one integrated iron and steel plant. In total, 19.78 Mio t CO2 (including impurities) are captured in the emitter cluster annually. The combined CO2 stream is transported in a trunk line with a length of 400 km (100 km of these offshore) and is injected into five generic storage structures. The storage reservoirs are saline aquifers of the Buntsandstein. The investigations revealed beneficial and deteriorating impacts of different impurities and combinations thereof. Overall, no fundamental technical obstacles for transporting, injecting and storing CO2 streams of the modelled variable compositions and mass flow rates were observed. Based on the results, the CLUSTER project team recommends not to define “minimum composition thresholds” for CO2 streams as strict threshold values for each individual impurity in the stream. Instead, CO2 stream compositions and variabilities for specific CCS projects should be constrained with regard to a set of parameters including i) the overall CO2 content, ii) maximum contents of relevant impurities or elements, iii) acceptable variability of CO2 stream composition, and iv) impurity combinations to be avoided. T2 - 15th International Conference on Greenhouse Gas Control Technologies, GHGT-15 CY - Online meeting DA - 15.03.2021 KW - Corrosion KW - Impurities KW - CO2 quality KW - Pipeline network KW - Whole-chain CCS scenario KW - Recommendations PY - 2021 DO - https://doi.org/10.2139/ssrn.3816427 SP - 1 EP - 18 AN - OPUS4-52418 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -