Aluminum foil negative electrodes with multiphase microstructure for all-solid-state Li-ion batteries

Yuhgene Liu; Congcheng Wang; Sun Geun Yoon; Sang Yun Han; John A Lewis; Dhruv Prakash; Emily J Klein; Timothy Chen; Dae Hoon Kang; Diptarka Majumdar; Rajesh Gopalaswamy; Matthew T McDowell

doi:10.1038/s41467-023-39685-x

Aluminum foil negative electrodes with multiphase microstructure for all-solid-state Li-ion batteries

Nat Commun. 2023 Jul 18;14(1):3975. doi: 10.1038/s41467-023-39685-x.

Authors

Affiliations

¹ School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
² George W. Woodruff School of Mechanical Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
³ Novelis, Inc., Kennesaw, GA, 30144, USA.
⁴ School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA. mattmcdowell@gatech.edu.
⁵ George W. Woodruff School of Mechanical Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA. mattmcdowell@gatech.edu.

Abstract

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 Al_94.5In_5.5 negative electrode is combined with a Li₆PS₅Cl solid-state electrolyte and a LiNi_0.6Mn_0.2Co_0.2O₂-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.