Title: Understanding the Effect of Interlayers at the Thiophosphate Solid Electrolyte/Lithium Interface for All-Solid-State Li Batteries

Abstract

All-solid-state Li-ion batteries afford possibilities to enhance battery safety while improving their energy and power densities. Current challenges for achieving high-performance all-solid-state batteries with long cycle life include shorting resulting predominantly from Li dendrite formation and infiltration through the solid electrolyte (SE) and increases in cell impedance induced by SE decomposition at the SE/electrode interface. In this work, we evaluate the electrochemical properties of two interlayer materials, Si and Li_xAl_(2-x/3)O₃ (LiAlO), at the Li₇P₃S₁₁ (LPS)/Li interface. Compared to the Li/LPS/Li symmetric cells in absence of interlayers, the presence of Si and LiAlO both significantly enhance the cycle number and total charge passing through the interface before failures resulting from cell shorting. In both cases, the noted improvements were accompanied by cell impedances that had increased substantially. The data reveal that both interlayers prevent the direct exposure of LPS to the metallic Li and therefore eliminate the intrinsic LPS decomposition that occurs at Li surfaces before electrochemical cycling. After cycling, a reduction of LPS to Li₂S occurs at the interface when a Si interlayer is present; LiAlO, which functions to drop the potential between Li and LPS, suppresses LPS decomposition processes. The relative propensities toward SE decomposition follows from the electrochemicalmore » potentials at the interface, which are dictated by the identities of the interlayer materials. As a result, this work provides new insights into the phase dynamics associated with specific choices for SE/electrode interlayer materials and the requirements they impose for realizing high efficiency, long lasting all-solid-state batteries.« less

Authors:

Sang, Lingzi ^[1]; Bassett, Kimberly L. ^[1]; Castro, Fernando C. ^[2]; Young, Matthias J.  ^[3];

• Search DOE PAGES for author "Young, Matthias J."
• Search DOE PAGES for ORCID "0000-0001-7384-4333"

Chen, Lin ^[3]; Haasch, Richard T.  ^[1];

• Search DOE PAGES for author "Haasch, Richard T."
• Search DOE PAGES for ORCID "0000-0001-9479-2595"

Elam, Jeffrey W.  ^[3];

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• Search DOE PAGES for ORCID "0000-0002-5861-2996"

Dravid, Vinayak P.  ^[2];

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• Search DOE PAGES for ORCID "0000-0002-6007-3063"

Nuzzo, Ralph G. ^[4]; Gewirth, Andrew A.  ^[1]

• Search DOE PAGES for author "Gewirth, Andrew A."
• Search DOE PAGES for ORCID "0000-0003-4400-9907"

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+ Show Author Affiliations

1. Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)
2. Northwestern Univ., Evanston, IL (United States)
3. Argonne National Lab. (ANL), Lemont, IL (United States)
4. Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States); KTH Royal Institute of Technology, Stockholm (Sweden)

Publication Date:

Fri Nov 30 00:00:00 EST 2018

Research Org.:

Energy Frontier Research Centers (EFRC) (United States). Center for Electrical Energy Storage (CEES); Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1500114

Grant/Contract Number:  

AC02-06CH11357

Resource Type:

Accepted Manuscript

Journal Name:

Chemistry of Materials

Additional Journal Information:

Journal Volume: 30; Journal Issue: 24; Journal ID: ISSN 0897-4756

Publisher:

American Chemical Society (ACS)

Country of Publication:

United States

Language:

English

Subject:

25 ENERGY STORAGE