TY - JOUR A1 - Tang, F. A1 - Li, D. A1 - Liu, X. A1 - Huang, H. A1 - Wu, C. A1 - Hilger, A. A1 - Markötter, Henning A1 - Wilde, F. A1 - Manke, I. A1 - Sun, F. A1 - Chen, L. T1 - Exploring optimal Li composite electrode anodes for lithium metal batteries through in situ X-ray computed tomography N2 - The uncontrolled Li dissolution/deposition dynamics and rapid Li pulverizations hinder the widespread deployment of Li metal batteries (LMB). Designing a Li composite electrode possessing a mechanically robust and lithiophilic three-dimensional (3D) framework represents a promising strategy to address these challenges. This study involves the preparation of three uniquely tailored Li-B-Mg composites using a combined metallurgical process of melting, casting, and rolling, along with the synergistic application of in situ X-ray computed tomography (CT) and post-mortem failure analysis to explore the most promising composite electrode candidate for LMBs. During the in-depth investigation, the optimal 70Li-B-Mg composite electrode stands out due to its robust skeleton fiber structure, uniform Li dissolution/deposition characteristics and high capacity of free-Li. Its promising prospects for enabling high-performance LMBs are showcased by the superior performance of the built Li||O2, Li||LiFePO4, Li||NCM622 and Li||NCM811 battery systems. This work offers a novel approach for exploring universally applicable and robust Li composite electrodes to realize high-performance LMBs using in situ CT analysis. KW - Li metal batteries KW - Li composite electrode KW - X-ray computed tomography KW - Li-B-Mg PY - 2024 DO - https://doi.org/10.1016/j.ensm.2024.103746 VL - 72 SP - 12 PB - Elsevier B.V. AN - OPUS4-61039 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - 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 -