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. 2025 Jul 9;17(27):39089-39096.
doi: 10.1021/acsami.5c06550. Epub 2025 Jun 25.

Effect of Silver Particle Distribution in a Carbon Nanocomposite Interlayer on Lithium Plating in Anode-Free All-Solid-State Batteries

Michael Metzler  1   2 , Christopher Doerrer  1   3 , Yige Sun  1   2 , Guillaume Matthews  1   2 , Enzo Liotti  1 , Patrick S Grant  1   2
Affiliations

Effect of Silver Particle Distribution in a Carbon Nanocomposite Interlayer on Lithium Plating in Anode-Free All-Solid-State Batteries

Michael Metzler et al. ACS Appl Mater Interfaces. .

Abstract

Solid-state batteries can outperform lithium-ion batteries in energy per unit mass or volume when operating with a Li metal anode. However, Li anodes pose significant manufacturing challenges. Anode-free cells avoid these challenges by plating metallic Li at the anode on the first charge, but subsequent nonuniform cyclic stripping and plating decrease the Coulombic efficiency and encourage Li dendrites and early cell failure. We report a new spray-printed nanocomposite bilayer of silver/carbon black (Ag/CB) between anodic current collectors and a Li6PS5Cl solid electrolyte comprising an Ag-rich region at the current collector and a CB-rich region at the solid electrolyte. Compared with previous Ag/CB mixtures, this bilayer promoted more uniform Li anode plating and improved cycling. Cells with a high-Ni oxide cathode had an initial discharge capacity of >190 mAh/g and a Coulombic efficiency of >98% over 100 cycles. Improved Li plating uniformity with the structured Ag/CB interlayer was confirmed by using secondary-ion mass spectrometry (SIMS) imaging.

Keywords: anode-free; battery structural design; layer-by-layer; secondary-ion mass spectrometry; silver−carbon layer; solid-state battery manufacturing; spray printing.

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Figures

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1
Summary of cell production. (a) Illustration of spray printing; (b) illustration of laser cutting; (c) illustration of the SSB full-cell arrangement; and (d) illustration of the three-electrode arrangement.
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SEM cross-section images of the spray printed (a) unstructured and (b) structured Ag/CB interlayers after uniaxial compression at 500 MPa; corresponding superimposed Ag and C EDS maps of the (c) unstructured and (d) structured interlayers. Green: Ag, Blue: C.
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Cycling of SSB cells with Ag/CB interlayers at 60 °C and 4 MPa stack pressure. (a) Voltage/time during single-charge tests of three-electrode cells with and without Ag/CB interlayers at 1 mA/cm2; (b) Voltage/capacity during the first charge/discharge cycle of full-cells with unstructured and structured Ag/CB interlayers at 1 mA/cm2 charge/discharge current; Long-term full-cell cycling stability with an (c) unstructured and (d) structured Ag/CB interlayer at 1 mA/cm2 charge/discharge current.
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Cross-section of the stainless-steel current collector, deposited layer, Ag/CB interlayer, and LPS separator region for a single charge at 2.5 mA/cm2. (a) SEM image of the structured Ag/CB; (b–e) EDS maps of S, C, Ag, and Fe respectively; (f) 7Li+ SIMS map; (g) SEM image of the unstructured Ag/CB interlayer; and (h, i) EDS maps of C and Fe, respectively.
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5
Schematic and idealized illustration of the Li plating mechanism upon charging for different Ag/CB interlayer arrangements. The plating mechanism for (a) unstructured and (b) structured Ag/CB interlayers.
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References

    1. Boaretto N., Garbayo I., Valiyaveettil-SobhanRaj S., Quintela A., Li C., Casas-Cabanas M., Aguesse F.. Lithium Solid-State Batteries: State-of-the-Art and Challenges for Materials, Interfaces and Processing. J. Power Sources. 2021;502:229919. doi: 10.1016/j.jpowsour.2021.229919. - DOI
    1. Waldmann T., Scurtu R.-G., Richter K., Wohlfahrt-Mehrens M.. 18650 vs. 21700 Li-Ion Cells–A Direct Comparison of Electrochemical, Thermal, and Geometrical Properties. J. Power Sources. 2020;472:228614. doi: 10.1016/j.jpowsour.2020.228614. - DOI
    1. Janek J., Zeier W.. A Solid Future for Battery Development. Nat. Energy. 2016;1(9):16141. doi: 10.1038/nenergy.2016.141. - DOI
    1. Betz J., Bieker G., Meister P., Placke T., Winter M., Schmuch R.. Theoretical versus Practical Energy: A Plea for More Transparency in the Energy Calculation of Different Rechargeable Battery Systems. Adv. Energy Mater. 2019;9(6):1803170. doi: 10.1002/aenm.201803170. - DOI
    1. Wood K., Noked M., Dasgupta N.. Lithium Metal Anodes: Toward an Improved Understanding of Coupled Morphological, Electrochemical, and Mechanical Behavior. ACS Energy Lett. 2017;2(3):664–672. doi: 10.1021/acsenergylett.6b00650. - DOI

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