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Title: Three-Dimensional Solid-State Lithium-Ion Batteries Fabricated by Conformal Vapor-Phase Chemistry

Abstract

Three-dimensional thin-film solid-state batteries (3D TSSB) were proposed by Long et al. in 2004 as a structure-based approach to simultaneously increase energy and power densities. Here, we report experimental realization of fully conformal 3D TSSBs, demonstrating the simultaneous power-and-energy benefits of 3D structuring. All active battery components—electrodes, solid electrolyte, and current collectors—were deposited by atomic layer deposition (ALD) onto standard CMOS processable silicon wafers microfabricated to form arrays of deep pores with aspect ratios up to approximately 10. The cells utilize an electrochemically prelithiated LiV2O5 cathode, a very thin (40–100 nm) Li2PO2N solid electrolyte, and a SnNx anode. The fabrication process occurs entirely at or below 250 °C, promising compatibility with a variety of substrates as well as integrated circuits. The multilayer battery structure enabled all-ALD solid-state cells to deliver 37 μAh/cm2·μm (normalized to cathode thickness) with only 0.02% per-cycle capacity loss. Conformal fabrication of full cells over 3D substrates increased the areal discharge capacity by an order of magnitude while simulteneously improving power performance, a trend consistent with a finite element model. Furthermore, this work shows that the exceptional conformality of ALD, combined with conventional semiconductor fabrication methods, provides an avenue for the successful realization of long-sought 3D TSSBsmore » which provide power performance scaling in regimes inaccessible to planar form factor cells.« less

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [1];  [2];  [3]; ORCiD logo [4];  [1];  [1]; ORCiD logo [1]
  1. Univ. of Maryland, College Park, MD (United States)
  2. American Society for Engineering Education, Washington, D.C. (United States)
  3. The Johns Hopkins Univ. Applied Physics Lab., Laurel, MD (United States)
  4. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-CA), Livermore, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Nanostructures for Electrical Energy Storage (NEES)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1464200
Report Number(s):
SAND-2018-8254J
Journal ID: ISSN 1936-0851; 666442
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 12; Journal Issue: 5; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; conformal battery; energy storage; solid-state battery; three-dimensional energy storage; three-dimensional solid-state battery

Citation Formats

Pearse, Alexander, Schmitt, Thomas, Sahadeo, Emily, Stewart, David M., Kozen, Alexander, Gerasopoulos, Konstantinos, Talin, Albert Alec, Lee, Sang Bok, Rubloff, Gary W., and Gregorczyk, Keith E. Three-Dimensional Solid-State Lithium-Ion Batteries Fabricated by Conformal Vapor-Phase Chemistry. United States: N. p., 2018. Web. doi:10.1021/acsnano.7b08751.
Pearse, Alexander, Schmitt, Thomas, Sahadeo, Emily, Stewart, David M., Kozen, Alexander, Gerasopoulos, Konstantinos, Talin, Albert Alec, Lee, Sang Bok, Rubloff, Gary W., & Gregorczyk, Keith E. Three-Dimensional Solid-State Lithium-Ion Batteries Fabricated by Conformal Vapor-Phase Chemistry. United States. https://doi.org/10.1021/acsnano.7b08751
Pearse, Alexander, Schmitt, Thomas, Sahadeo, Emily, Stewart, David M., Kozen, Alexander, Gerasopoulos, Konstantinos, Talin, Albert Alec, Lee, Sang Bok, Rubloff, Gary W., and Gregorczyk, Keith E. 2018. "Three-Dimensional Solid-State Lithium-Ion Batteries Fabricated by Conformal Vapor-Phase Chemistry". United States. https://doi.org/10.1021/acsnano.7b08751. https://www.osti.gov/servlets/purl/1464200.
@article{osti_1464200,
title = {Three-Dimensional Solid-State Lithium-Ion Batteries Fabricated by Conformal Vapor-Phase Chemistry},
author = {Pearse, Alexander and Schmitt, Thomas and Sahadeo, Emily and Stewart, David M. and Kozen, Alexander and Gerasopoulos, Konstantinos and Talin, Albert Alec and Lee, Sang Bok and Rubloff, Gary W. and Gregorczyk, Keith E.},
abstractNote = {Three-dimensional thin-film solid-state batteries (3D TSSB) were proposed by Long et al. in 2004 as a structure-based approach to simultaneously increase energy and power densities. Here, we report experimental realization of fully conformal 3D TSSBs, demonstrating the simultaneous power-and-energy benefits of 3D structuring. All active battery components—electrodes, solid electrolyte, and current collectors—were deposited by atomic layer deposition (ALD) onto standard CMOS processable silicon wafers microfabricated to form arrays of deep pores with aspect ratios up to approximately 10. The cells utilize an electrochemically prelithiated LiV2O5 cathode, a very thin (40–100 nm) Li2PO2N solid electrolyte, and a SnNx anode. The fabrication process occurs entirely at or below 250 °C, promising compatibility with a variety of substrates as well as integrated circuits. The multilayer battery structure enabled all-ALD solid-state cells to deliver 37 μAh/cm2·μm (normalized to cathode thickness) with only 0.02% per-cycle capacity loss. Conformal fabrication of full cells over 3D substrates increased the areal discharge capacity by an order of magnitude while simulteneously improving power performance, a trend consistent with a finite element model. Furthermore, this work shows that the exceptional conformality of ALD, combined with conventional semiconductor fabrication methods, provides an avenue for the successful realization of long-sought 3D TSSBs which provide power performance scaling in regimes inaccessible to planar form factor cells.},
doi = {10.1021/acsnano.7b08751},
url = {https://www.osti.gov/biblio/1464200}, journal = {ACS Nano},
issn = {1936-0851},
number = 5,
volume = 12,
place = {United States},
year = {2018},
month = {4}
}

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Cited by: 6 works
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Figures / Tables:

Figure 1 Figure 1: Methods of improving energy storage metrics for thin film solid state batteries. Increasing the electrode thickness scales energy density at the expense of power density due to the rapid increase in the characteristic diffusion time for ions in the thick electrode. Fabricating TSSBs in a 3D structure bothmore » increases areal material loading and increases power performance through a decrease in the internal current density due to the larger internal surface area.« less

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Works referenced in this record:

All-Solid-State Lithium-Ion Microbatteries: A Review of Various Three-Dimensional Concepts
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Solid-state thin-film rechargeable batteries
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All-Solid-State Lithium-Ion Microbatteries Using Silicon Nanofilm Anodes: High Performance and Memory Effect
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Electrochemical Thin Layers in Nanostructures for Energy Storage
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Lithium Diffusion in Li[sub x]CoO[sub 2] (0.45 < x < 0.7) Intercalation Cathodes
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Works referencing / citing this record:

Advances in 3D Thin‐Film Li‐Ion Batteries
journal, June 2019


Tape‐Casting Li 0.34 La 0.56 TiO 3 Ceramic Electrolyte Films Permit High Energy Density of Lithium‐Metal Batteries
journal, November 2019


Atomic layer deposition and first principles modeling of glassy Li 3 BO 3 –Li 2 CO 3 electrolytes for solid-state Li metal batteries
journal, January 2018


Reducing the Interfacial Resistance in All‐Solid‐State Lithium Batteries Based on Oxide Ceramic Electrolytes
journal, April 2019


Plasma-Assisted ALD of LiPO(N) for Solid State Batteries
journal, January 2019


Figures / Tables found in this record:

2O5/50nm Li2PO2N / lOnm SnNx/ 25nm TiN. (i) Overview of ALD chemistry and process temperature for each layer visible in (h)." data-ostiid="1464200" style="padding-bottom: 2em; border-bottom: 1px solid #ddd;">
Figure 2(p. 4)figure
Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.