Title: F and N Rich Solid Electrolyte for Stable All-Solid-State Battery

Abstract

Abstract The instability of sulfide solid electrolytes to Li anode and high‐voltage LiNi _0.8 Mn _0.1 Co _0.1 O ₂ (NMC811) cathodes limits the cyclic performance of all‐solid‐state lithium battery (ASSLB). Herein, the stability of Li ₆ PS ₅ Cl against Li anode is enhanced by mixing a small amount (0.32 wt%) of CuF ₂ ‐LiNO ₃ (CL) into Li ₆ PS ₅ Cl electrolyte layer to in‐situ form a mixed‐conductive‐lithiophobic and self‐healing LiF‐Li ₃ N‐Cu solid electrolyte interphase (SEI) at Li ₆ PS ₅ Cl‐CL/Li interface. The critical current density (CCD) of Li ₆ PS ₅ Cl‐CuF ₂ ‐LiNO ₃ increases to 1.4 mA cm ^–2 /1.4 mAh cm ^–2 at room temperature, which is much higher than that of pristine Li ₆ PS ₅ Cl (0.4 mA cm ^–2 /0.4 mAh cm ^–2 ) even though mixing 0.32 wt% CL into Li ₆ PS ₅ Cl slightly reduces the ionic conductivity from 2.9 × 10 ^–3 to 1.5 × 10 ^–3 S cm ^–1 . The compatibility of Li ₆ PS ₅ Cl‐CL electrolyte to single‐crystalline NMC811 (S‐NMC811) is further enhanced by adding a small amount (0.02 wt%) of AlF ₃ into Li ₆ PS ₅ Cl‐CL forming Li ₆ PS ₅ Cl‐CuF ₂ ‐LiNO ₃more » ‐AlF ₃ (Li ₆ PS ₅ Cl‐CLA) as a cathode electrolyte and by doing Cl ^– on S‐NMC811 (Cl@S‐NMC811) surface. The Cl@S‐NMC811‐Li ₆ PS ₅ Cl‐CLA|Li ₆ PS ₅ Cl‐CL|Li cells with areal capacity of 2.55 mAh cm ^‐2 achieve a capacity retention of 69.4% after 100 cycles at 1C (1C = 200 mAh g ^‐1 ). Adding a small amount of SEI and cathode/electrolyte interphase (CEI) former into the sulfide electrolytes with minimal reduction (48.3%) of ionic conductivity is an effective method to enhance the performance of ASSLB.« less

Authors:

Wan, Hongli L. ^[1]; Zhang, Jiaxun X. ^[1]; Xia, Jiale L. ^[1]; Ji, Xiao ^[1]; He, Xinzi Z. ^[1]; Liu, Sufu F. ^[1]; Wang, Chunsheng S.  ^[1]

• Search DOE PAGES for author "Wang, Chunsheng S."
• Search DOE PAGES for ORCID "0000-0002-8626-6381"

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+ Show Author Affiliations

1. University of Maryland, College Park, MD (United States)

Publication Date:

Sun Dec 26 00:00:00 EST 2021

Research Org.:

Univ. of California, San Diego, CA (United States); Univ. of Maryland, College Park, MD (United States)

Sponsoring Org.:

USDOE Advanced Research Projects Agency - Energy (ARPA-E)

OSTI Identifier:

1976185

Alternate Identifier(s):

OSTI ID: 1837707

Grant/Contract Number:  

AR0000781; EE0008856; DEEE0008856

Resource Type:

Accepted Manuscript

Journal Name:

Advanced Functional Materials

Additional Journal Information:

Journal Volume: 32; Journal Issue: 15; Journal ID: ISSN 1616-301X

Publisher:

Wiley

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; all-solid-state lithium battery; single-crystalline LiNi0.8Co0.1Mn0.1O2; halogen doping; solidelectrolyte interphase; cathode/electrolyte interphase