Scaling-Up Insights for Zinc–Air Battery Technologies Realizing Reversible Zinc Anodes Advanced Materials, Early View https://doi.org/10.1002/adma.202303509 Sambhaji S. Shinde, Nayantara K. Wagh, Chi Ho Lee, Dong-Hyung Kim, Sung-Hae Kim, Han-Don Um, Sang Uck Lee, Jung-Ho Lee Abstract Zinc–air battery (ZAB) technology is considered one of the promising candidates to complement the existing lithium-ion batteries for future large-scale high-energy-storage demands. The scientific literature reveals many efforts for the ZAB chemistries, materials design, and limited accounts for cell design principles with apparently superior performances for liquid and solid-state electrolytes. However, along with the difficulty of forming robust solid-electrolyte interphases, the discrepancy in testing methods and assessment metrics severely challenges the realistic evaluation/comparison and commercialization of ZABs. Here, strategies to formulate reversible zinc anodes are proposed and specific cell-level energy metrics (100−500 Wh kg−1) and realistic long-cycling operations are realized. Stabilizing anode/electrolyte interfaces results in a cumulative capacity of 25 Ah cm−2 and Coulomb efficiency of >99.9% for 5000 plating/stripping cycles. Using 1–10 Ah scale (≈500 Wh kg−1 at cell level) solid-state zinc–air pouch cells, scale-up insights for Ah-level ZABs that can progress from lab-scale research to practical production are also offered.

Li, Na, K, Mg, Zn, Al, and Ca Anode Interface Chemistries Developed by Solid-State Electrolytes Advanced Science, Early View, 2304235 https://doi.org/10.1002/advs.202304235 Sambhaji S. Shinde, Nayantara K. Wagh, Sung-Hae Kim, Jung-Ho Lee Abstract Solid-state batteries (SSBs) have received significant attention due to their high energy density, reversible cycle life, and safe operations relative to commercial Li-ion batteries using flammable liquid electrolytes. This review presents the fundamentals, structures, thermodynamics, chemistries, and electrochemical kinetics of desirable solid electrolyte interphase (SEI) required to meet the practical requirements of reversible anodes. Theoretical and experimental insights for metal nucleation, deposition, and stripping for the reversible cycling of metal anodes are provided. Ion transport mechanisms and state-of-the-art solid-state electrolytes (SEs) are discussed for realizing high-performance cells. The interface challenges and strategies are also concerned with the integration of SEs, anodes, and cathodes for large-scale SSBs in terms of physical/chemical contacts, space-charge layer, interdiffusion, lattice-mismatch, dendritic growth, chemical reactivity of SEI, current collectors, and thermal instability. The recent innovations for anode interface chemistries developed by SEs are highlighted with monovalent (lithium (Li+), sodium (Na+), potassium (K+)) and multivalent (magnesium (Mg2+), zinc (Zn2+), aluminum (Al3+), calcium (Ca2+)) cation carriers (i.e., lithium-metal, lithium-sulfur, sodium-metal, potassium-ion, magnesium-ion, zinc-metal, aluminum-ion, and calcium-ion batteries) compared to those of liquid counterparts.

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