TY - JOUR A1 - Bloi, L. M. A1 - Hippauf, F. A1 - Boenke, T. A1 - Rauche, M. A1 - Paasch, S. A1 - Schutjajew, K. A1 - Pampel, Jonas A1 - Schwotzer, F. A1 - Dörfler, S. A1 - Althues, H. A1 - Oschatz, M. A1 - Brunner, E. A1 - Kaskel, S. T1 - Mechanistic insights into the reversible lithium storage in an open porous carbon via metal cluster formation in all solid-state batteries N2 - Porous carbons are promising anode materials for next generation lithium batteries due to their large lithium storage capacities. However, their highsloping capacity during lithiation and delithiation as well as capacity fading due to intense formation of solid electrolyte interphase (SEI) limit their gravimetric and volumetric energy densities. Herein we compare a microporous carbide-derived carbon material (MPC) as promising future anode for all solid-state batteries with a commercial high-performance hard carbon anode. The MPC obtains high and reversible lithiation capacities of 1000 mAh g−1carbon in half-cells exhibiting an extended plateau region near 0 V vs. Li/Li+ preferable for full-cell application. The well-defined microporosity of the MPC with a specific surface area of >1500 m2 g−1 combines well with the argyrodite-type electrolyte (Li6PS5Cl) suppressing extensive SEI formation to deliver high coulombic efficiencies. Preliminary full-cell measurements vs. nickel-rich NMC-cathodes (LiNi0.9Co0.05Mn0.05O2) provide a considerably improved average potential of 3.76 V leading to a projected energy density as high as 449 Wh kg−1 and reversible cycling for more than 60 cycles. 7Li Nuclear Magnetic Resonance spectroscopy was combined with ex-situ Small Angle X-ray Scattering to elucidate the storage mechanism of lithium inside the carbon matrix. The formation of extended quasi-metallic lithium clusters after electrochemical lithiation was revealed. KW - All solid-state battery KW - Microporous carbon KW - Lithium battery KW - Anode PY - 2022 DO - https://doi.org/10.1016/j.carbon.2021.11.061 SN - 0008-6223 VL - 188 SP - 325 EP - 335 PB - Elsevier Ltd. AN - OPUS4-54079 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 - Debatin, F. A1 - Behrens, K. A1 - Weber, J. A1 - Baburin, I. A. A1 - Thomas, A. A1 - Schmidt, J. A1 - Senkovska, I. A1 - Kaskel, S. A1 - Kelling, A. A1 - Hedin, N. A1 - Bacsik, Z. A1 - Leoni, S. A1 - Seifert, G. A1 - Jäger, Christian A1 - Günter, C. A1 - Schilde, U. A1 - Friedrich, A. A1 - Holdt, H.-J. T1 - An isoreticular family of microporous metal-organic frameworks based on zinc and 2-substituted imidazolate-4-amide-5-imidate: syntheses, structures and properties N2 - We report on a new series of isoreticular frameworks based on zinc and 2-substituted imidazolate-4-amide-5-imidate (IFP-1–4, IFP=imidazolate framework Potsdam) that form one-dimensional, microporous hexagonal channels. Varying R in the 2-substitued linker (R=Me (IFP-1), Cl (IFP-2), Br (IFP-3), Et (IFP-4)) allowed the channel diameter (4.0–1.7 Å), the polarisability and functionality of the channel walls to be tuned. Frameworks IFP-2, IFP-3 and IFP-4 are isostructural to previously reported IFP-1. The structures of IFP-2 and IFP-3 were solved by X-ray crystallographic analyses. The structure of IFP-4 was determined by a combination of PXRD and structure modelling and was confirmed by IR spectroscopy and 1H MAS and 13C CP-MAS NMR spectroscopy. All IFPs showed high thermal stability (345–400°C); IFP-1 and IFP-4 were stable in boiling water for 7 d. A detailed porosity analysis was performed on the basis of adsorption measurements by using various gases. The potential of the materials to undergo specific interactions with CO2 was investigated by measuring the isosteric heats of adsorption. The capacity to adsorb CH4 (at 298 K), CO2 (at 298 K) and H2 (at 77 K) at high pressure were also investigated. In situ IR spectroscopy showed that CO2 is physisorbed on IFP-1–4 under dry conditions and that both CO2 and H2O are physisorbed on IFP-1 under moist conditions. KW - Adsorption KW - Metal-organic frameworks KW - Microporous materials KW - N,O ligands KW - Zinc PY - 2012 DO - https://doi.org/10.1002/chem.201200889 SN - 0947-6539 SN - 1521-3765 VL - 18 IS - 37 SP - 11630 EP - 11640 PB - Wiley-VCH Verl. CY - Weinheim AN - OPUS4-27725 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Debatin, F. A1 - Thomas, A. A1 - Kelling, A. A1 - Hedin, N. A1 - Bacsik, Z. A1 - Senkovska, I. A1 - Kaskel, S. A1 - Junginger, M. A1 - Müller, H. A1 - Schilde, U. A1 - Jäger, Christian A1 - Friedrich, A. A1 - Holdt, H.-J. T1 - In situ synthesis of an imidazolate-4-amide-5-imidate ligand and formation of a microporous zinc-organic framework with H2-and CO2-storage ability KW - Metal-organic framework KW - Synthesis KW - XRD KW - FTIR KW - NMR KW - Gas sorption KW - Microporous materials KW - N,O ligands KW - Solvothermal synthesis PY - 2010 DO - https://doi.org/10.1002/anie.200906188 SN - 1433-7851 SN - 1521-3773 SN - 0570-0833 VL - 49 IS - 7 SP - 1258 EP - 1262 PB - Wiley-VCH CY - Weinheim AN - OPUS4-21132 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -