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  1. 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 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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  3. Lithium metal and lithium-rich alloys are high-capacity anode materials that could boost the energy content of rechargeable batteries. However, their development has been hindered by rapid capacity decay during cycling, which is driven by the substantial structural, morphological, and volumetric transformations that these materials and their interfaces experience during charge and discharge. During these transformations, the interplay between chemical/structural changes and solid mechanics plays a defining role in determining electrochemical degradation. This Perspective discusses how chemistry and mechanics are interrelated in influencing the reaction mechanisms, stability, and performance of both lithium metal anodes and alloy anodes. Battery systems with liquid electrolytes and solid-state electrolytes are considered because of the distinct effects of chemo-mechanics in each system. Building on this knowledge, we present a discussion of emerging ideas to control and mitigate chemo-mechanical degradation in these materials to enable translation to commercial systems, which could lead to the development of high-energy batteries that are urgently needed to power our increasingly electrified world. 
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  4. null (Ed.)