TY - JOUR A1 - Lu, J. A1 - Zhang, S. A1 - Yao, J. A1 - Guo, Z. A1 - Osenberg, M. A1 - Hilger, A. A1 - Markötter, Henning A1 - Wilde, F. A1 - Manke, I. A1 - Zhang, X. A1 - Sun, F. A1 - Cui, G. T1 - Synergistic Effect of CO2 in Accelerating the Galvanic Corrosion of Lithium/Sodium Anodes in Alkali Metal−Carbon Dioxide Batteries N2 - Rechargeable alkali metal−CO2 batteries, which combine high theoretical energy density and environmentally friendly CO2 fixation ability, have attracted worldwide attention. Unfortunately, their electrochemical performances are usually inferior for practical applications. Aiming to reveal the underlying causes, a combinatorial usage of advanced nondestructive and postmortem characterization tools is used to intensively study the failure mechanisms of Li/Na−CO2 batteries. It is found that a porous interphase layer is formed between the separator and the Li/Na anode during the overvoltage rising and battery performance decaying process. A series of control experiments are designed to identify the underlying mechanisms dictating the observed morphological evolution of Li/Na anodes, and it is found that the CO2 synergist facilitates Li/Na chemical corrosion, the process of which is further promoted by the unwanted galvanic corrosion and the electrochemical cycling conditions. A detailed compositional analysis reveals that the as-formed interphase layers under different conditions are similar in species, with the main differences being their inconsistent quantity. Theoretical calculation results not only suggest an inherent intermolecular affinity between the CO2 and the electrolyte solvent but also provide the most thermodynamically favored CO2 reaction pathways. Based on these results, important implications for the further development of rechargeable alkali metal−CO2 batteries are discussed. The current discoveries not only fundamentally enrich our knowledge of the failure mechanisms of rechargeable alkali metal−CO2 batteries but also provide mechanistic directions for protecting metal anodes to build high-reversible alkali metal−CO2 batteries. KW - Alkali metal batteries KW - Synchrotron X-ray computed tomography KW - Lithium/sodium−carbon dioxide batteries KW - Battery failure mechanisms KW - Alkali metal anodes PY - 2024 DO - https://doi.org/10.1021/acsnano.4c02329 SP - 1 EP - 16 AN - OPUS4-59922 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 - 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 - Krüger, P. A1 - Markötter, Henning A1 - Klages, M. A1 - Haußmann, J. A1 - Arlt, Tobias A1 - Riesemeier, Heinrich A1 - Hartnig, C. A1 - Banhart, J. A1 - Manke, I. A1 - Scholta, J. T1 - Dreidimensionale Untersuchung der Wasserverteilung in einer Miniatur-PEM-Brennstoffzelle KW - Resolution neutron-radiography KW - Local current distribution KW - Cells KW - Quantification PY - 2010 SN - 0025-5300 VL - 52 IS - 10 SP - 712 EP - 717 PB - Hanser CY - München AN - OPUS4-23044 LA - deu AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Al-Falahat, A.M. A1 - Kupsch, Andreas A1 - Hentschel, M.P. A1 - Lange, A. A1 - Kardjilov, N. A1 - Markötter, Henning A1 - Manke, I. T1 - Correction approach of detector backlighting in radiography N2 - In various kinds of radiography, deficient transmission imaging may occur due to backlighting inside the detector itself arising from light or radiation scattering. The related intensity mismatches barely disturb the high resolution contrast, but its long range nature results in reduced attenuation levels which are often disregarded. Based on X-ray observations and an empirical formalism, a procedure is developed for a first order correction of detector backlighting. A backlighting factor is modeled as a function of the relative detector coverage by the sample projection. Different cases of sample transmission are regarded at different backlight factors and detector coverage. The additional intensity of backlighting may strongly affect the values of materials’ attenuation up to a few 10%. The presented scenario provides a comfortable procedure for corrections of X-ray or neutron transmission imaging data. KW - X-ray imaging KW - Neutron imaging KW - Radiology KW - Backlighting KW - Digital detector array PY - 2019 DO - https://doi.org/10.1063/1.5097170 SN - 0034-6748 VL - 90 IS - 12 SP - 125108 PB - American Institute of Physics CY - Melville, NY, USA AN - OPUS4-50217 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Markötter, Henning A1 - Alink, R. A1 - Haußmann, J. A1 - Dittmann, K. A1 - Arlt, Tobias A1 - Wieder, F. A1 - Tötzke, C. A1 - Klages, M. A1 - Reiter, C. A1 - Riesemeier, Heinrich A1 - Scholta, J. A1 - Gerteisen, D. A1 - Banhart, J. A1 - Manke, I. T1 - Visualization of the water distribution in perforated gas diffusion layers by means of synchrotron X-ray radiography N2 - Perforated gas diffusion layers (GDLs) of polymer electrolyte membrane fuel cells (PEMFCs) were investigated by means of in-situ synchrotron X-ray radiography during operation. We found a strong influence of perforations on the water distribution and transport in the investigated Toray TGP-H-090 GDL. The water occurs mainly around the perforations, while the holes themselves show varying water distributions. Some remain dry, while most of them fill up with liquid water after a certain period or might serve as drainage volume for effective water transport. KW - Polymer electrolyte membrane fuel cell (PEMFC) KW - Radiography KW - Synchrotron KW - X-ray imaging KW - Perforated gas diffusion layer (GDL) KW - Water transport PY - 2012 DO - https://doi.org/10.1016/j.ijhydene.2012.01.141 SN - 0360-3199 VL - 37 IS - 9 SP - 7757 EP - 7761 PB - Elsevier CY - Oxford AN - OPUS4-26434 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Williams, S. H. A1 - Hilger, A. A1 - Kardjilov, N. A1 - Manke, I. A1 - Strobl, M. A1 - Douissard, P.A. A1 - Martin, T. A1 - Riesemeier, Heinrich A1 - Banhart, J. T1 - Detection system for microimaging with neutrons N2 - A new high-resolution detector setup for neutron imaging has been developed based on infinity-corrected optics with high light collection, combined with customized mounting hardware. The system can easily be installed, handled and fitted to any existing facility, avoiding the necessity of complex optical systems or further improved electronics (CCD). This is the first time optical magnification higher than 1:1 has been used with scintillator-based neutron detectors, as well as the first implementation of infinity corrected optics for neutron imaging, achieving the smallest yet reported effective pixel size of 3.375 µm. A novel transparent crystal scintillator (GGG crystal) has been implemented with neutrons for the first time to overcome limitations of traditional powder scintillators (Li6/ZnS, Gadox). The standardized procedure for resolution measurements with the Modulation Transfer Function (MTF) is summarized to facilitate comparison between instruments and facilities. Using this new detector setup, a resolution of 14.8 µm with a field of view of 6 mm × 6 mm has been achieved while maintaining reasonable count times. These advances open a wide range of new possible research applications and allow the potential for additional future developments. KW - Instrumentation for neutron sources KW - Neutron radiography KW - Neutron detectors (cold, thermal, fast neutrons) PY - 2012 DO - https://doi.org/10.1088/1748-0221/7/02/P02014 SN - 1748-0221 VL - 7 IS - P02014 SP - 1 EP - 26 PB - Inst. of Physics Publ. CY - London AN - OPUS4-26433 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Griesche, Axel A1 - Dabah, Eitan A1 - Kannengießer, Thomas A1 - Hilger, A. A1 - Kardjilov, N. A1 - Manke, I. A1 - Schillinger, B. T1 - Measuring hydrogen distributions in iron and steel using neutrons N2 - Neutron tomography has been applied to investigate the mechanism of hydrogen assisted cracking in technical iron and supermartensitic steel. Rectangular technical iron block samples showed blistering due to intense hydrogen charging and the tomographic method revealed in situ the spatial distribution of hydrogen and cracks. Hydrogen accumulated in a small region around cracks and the cracks are filled with hydrogen gas. Cracks close to the surface contained no hydrogen. Hydrogenous tensile test samples of supermartensitic steel were pulled until rupture and showed hydrogen accumulations at the notch base and in the plastically deformed region around the fracture surface. T2 - 10th World Conference on Neutron Radiography (WCNR) CY - Grindelwald, Switzerland DA - 05.10.2014 PY - 2015 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-348022 DO - https://doi.org/10.1016/j.phpro.2015.07.062 SN - 1875-3892 VL - 69 SP - 445 EP - 450 PB - Elsevier B.V. CY - Amsterdam AN - OPUS4-34802 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Markötter, Henning A1 - Manke, I. A1 - Haußmann, J. A1 - Arlt, Tobias A1 - Klages, M. A1 - Krüger, P. A1 - Hartnig, C. A1 - Scholta, J. A1 - Müller, Bernd R. A1 - Riesemeier, Heinrich A1 - Banhart, J. T1 - Combined synchrotron X-ray radiography and tomography study of water transport in gas diffusion layers N2 - Synchrotron X-ray radiography and tomography investigations of a custom-made polymer electrolyte membrane fuel cell optimised for visualisation purposes are presented. The 3D water distribution and transport pathways in the porous carbon fibre gas diffusion layers (GDLs) were investigated. The authors found that water is not only moving from the GDL into the channel, but can also take the opposite way, that is, from the channel into free pore space of the GDL. Such movement of water into the opposite direction has been subject of speculations but has so far not yet been reported and might bring new insights into the general water transport behaviour, which might give new aspects to the general description of water transport processes and influence modelling assumptions to describe the process taking place in the GDL. KW - Synchrotron radiography KW - Synchrotron tomography KW - Gas diffusion layers KW - Water transport PY - 2012 DO - https://doi.org/10.1049/mnl.2012.0410 SN - 1750-0443 VL - 7 IS - 7 SP - 689 EP - 692 PB - IET CY - London AN - OPUS4-26282 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 -