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Synergistic Effect of CO2 in Accelerating the Galvanic Corrosion of Lithium/Sodium Anodes in Alkali Metal−Carbon Dioxide Batteries

  • 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 detailedRechargeable 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.zeige mehrzeige weniger

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Metadaten
Autor*innen:J. Lu, S. Zhang, J. Yao, Z. Guo, M. Osenberg, A. Hilger, Henning Markötter, F. Wilde, I. Manke, X. Zhang, F. Sun, G. Cui
Dokumenttyp:Zeitschriftenartikel
Veröffentlichungsform:Verlagsliteratur
Sprache:Englisch
Titel des übergeordneten Werkes (Englisch):ACS Nano
Jahr der Erstveröffentlichung:2024
Organisationseinheit der BAM:8 Zerstörungsfreie Prüfung
8 Zerstörungsfreie Prüfung / 8.5 Röntgenbildgebung
Aufsatznummer:02329
Erste Seite:1
Letzte Seite:16
DDC-Klassifikation:Technik, Medizin, angewandte Wissenschaften / Ingenieurwissenschaften / Angewandte Physik
Freie Schlagwörter:Alkali metal anodes; Alkali metal batteries; Battery failure mechanisms; Lithium/sodium−carbon dioxide batteries; Synchrotron X-ray computed tomography
Themenfelder/Aktivitätsfelder der BAM:Energie
Energie / Elektrische Energiespeicher und -umwandlung
DOI:10.1021/acsnano.4c02329
Verfügbarkeit des Dokuments:Datei im Netzwerk der BAM verfügbar ("Closed Access")
Datum der Freischaltung:22.04.2024
Referierte Publikation:Ja
Datum der Eintragung als referierte Publikation:22.04.2024
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