Metal negative electrodes that alloy with lithium have high theoretical charge storage capacity and are ideal candidates for developing high-energy rechargeable batteries. However, such electrode materials show limited reversibility in Li-ion batteries with standard non-aqueous liquid electrolyte solutions. To circumvent this issue, here we report the use of non-pre-lithiated aluminum-foil-based negative electrodes with engineered microstructures in an all-solid-state Li-ion cell configuration. When a 30-μm-thick Al94.5In5.5negative electrode is combined with a Li6PS5Cl solid-state electrolyte and a LiNi0.6Mn0.2Co0.2O2-based positive electrode, lab-scale cells deliver hundreds of stable cycles with practically relevant areal capacities at high current densities (6.5 mA cm−2). We also demonstrate that the multiphase Al-In microstructure enables improved rate behavior and enhanced reversibility due to the distributed LiIn network within the aluminum matrix. These results demonstrate the possibility of improved all-solid-state batteries via metallurgical design of negative electrodes while simplifying manufacturing processes.
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Lee, Chanhee ; Han, Sang Yun ; Lewis, John A. ; Shetty, Pralav P. ; Yeh, David ; Liu, Yuhgene ; Klein, Emily ; Lee, Hyun-Wook ; McDowell, Matthew T. ( , ACS Energy Letters)null (Ed.)
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Han, Sang Yun ; Lewis, John A. ; Shetty, Pralav P. ; Tippens, Jared ; Yeh, David ; Marchese, Thomas S. ; McDowell, Matthew T. ( , Chemistry of Materials)
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Lewis, John A. ; Cortes, Francisco Javier ; Liu, Yuhgene ; Miers, John C. ; Verma, Ankit ; Vishnugopi, Bairav S. ; Tippens, Jared ; Prakash, Dhruv ; Marchese, Thomas S. ; Han, Sang Yun ; et al ( , Nature Materials)null (Ed.)