Abstract

Abstract All‐solid‐state batteries suffer from high interface resistance and lithium dendrite growth leading to low Li plating/stripping Coulombic efficiency (CE) of <90% and low critical current density at high capacity. Here, simultaneously addresses both challenges are simultaneously addressed and the Li plating/stripping CE is significantly increased to 99.6% at 0.2 mA cm ⁻² /0.2 mAh cm ⁻² , and critical current density (CCD) of > 3.0 mA cm ⁻² /3.0 mAh cm ⁻² by inserting a mixed ionic‐electronic conductive (MIEC) and lithiophobic LiF‐C‐Li ₃ N‐Bi nanocomposite interlayer between Li ₆ PS ₅ Cl electrolyte and Li anode. The highly lithiophobic LiF‐C‐Li ₃ N‐Bi interlayer with high ionic conductivity (10 ⁻⁵  S cm ⁻¹ ) and low electronic conductivity (3.4×10 ⁻⁷  S cm ⁻¹ ) enables Li to plate on the current collector (CC) surface rather than on Li ₆ PS ₅ Cl surface avoiding Li ₆ PS ₅ Cl electrolyte reduction. During initial Li plating on CC, Li penetrates into porous LiF‐C‐Li ₃ N‐Bi interlayer and lithiates Bi nanoparticles into Li ₃ Bi. The lithiophilic Li ₃ Bi and Li ₃ N nanoparticles in LiF‐C‐Li ₃ N‐Li ₃ Bi sub‐interlayer will move to CC along with plated Li, forming LiF‐C/Li ₃ N‐Li ₃ Bi lithiophobic/lithiophilic sublayer during the following Limore » stripping. This interlayer enables Co _0.1 Fe _0.9 S ₂ /Li ₆ PS ₅ Cl/Li cell with an areal capacity of 1.4 mAh cm ⁻² to achieve a cycle life of >850 cycles at 150 mA g ⁻¹ . The lithiophobic/lithiophilic interlayer enables solid‐state metal batteries to simultaneously achieve high energy and long cycle life.« less

Authors:

Wan, Hongli  ^[1];

• Search DOE PAGES for author "Wan, Hongli"
• Search DOE PAGES for ORCID "0009-0002-8115-0336"

Zhang, Bao ^[2]; Liu, Sufu ^[1]; Wang, Zeyi ^[1]; Xu, Jijian ^[1]; Wang, Chunsheng  ^[1]

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

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+ Show Author Affiliations

1. Department of Chemical and Biomolecular Engineering University of Maryland College Park MD 20740 USA
2. School of Physical and Mathematical Sciences Nanyang Technological University Singapore 637371 Singapore

Publication Date:

Fri Dec 29 00:00:00 EST 2023

Sponsoring Org.:

USDOE

OSTI Identifier:

2267595

Grant/Contract Number:  

DEEE0008856

Resource Type:

Publisher's Accepted Manuscript

Journal Name:

Advanced Energy Materials

Additional Journal Information:

Journal Name: Advanced Energy Materials; Journal ID: ISSN 1614-6832

Publisher:

Wiley Blackwell (John Wiley & Sons)

Country of Publication:

Germany

Language:

English