Title: Novel ALD Chemistry Enabled Low-Temperature Synthesis of Lithium Fluoride Coatings for Durable Lithium Anodes

Abstract

Lithium metal anodes can largely enhance the energy density of rechargeable batteries because of the high theoretical capacity and the high negative potential. However, the problem of lithium dendrite formation and low Coulombic efficiency (CE) during electrochemical cycling must be solved before lithium anodes can be widely deployed. Herein, a new atomic layer deposition (ALD) chemistry to realize the low-temperature synthesis of homogeneous and stoichiometric lithium fluoride (LiF) is reported, which then for the first time, as far as we know, is deposited directly onto lithium metal. The LiF preparation is performed at 150 degrees C yielding 0.8 angstrom/cycle. The LiF films are found to be crystalline, highly conformal, and stoichiometric with purity levels >99%. Nanoindentation measurements demonstrate the LiF achieving a shear modulus of 58 GPa, 7 times higher than the sufficient value to resist lithium dendrites. When used as the protective coating on lithium, it enables a stable Coulombic efficiency as high as 99.5% for over 170 cycles, about 4 times longer than that of bare lithium anodes. The remarkable battery performance is attributed to the nanosized LiF that serves two critical functions simultaneously: (1) the high dielectric value creates a uniform current distribution for excellent lithium stripping/platingmore » and ultrahigh mechanical strength to suppress lithium dendrites; (2) the great stability and electrolyte isolation by the pure LiF on lithium prevents parasitic reactions for a much improved CE. This new ALD chemistry for conformal LiF not only offers a promising avenue to implement lithium metal anodes for high-capacity batteries but also paves the way for future studies to investigate failure and evolution mechanisms of solid electrolyte interphase (SEI) using our LiF on anodes such as graphite, silicon, and lithium.« less

Authors:

Chen, Lin ^[1]; Chen, Kan -Sheng ^[2]; Chen, Xinjie ^[2]; Ramirez, Giovanni ^[3]; Huang, Zhennan ^[4]; Geise, Natalie R. ^[5]; Steinrück, Hans -Georg ^[6]; Fisher, Brandon L. ^[1]; Shahbazian-Yassar, Reza ^[4]; Toney, Michael F.  ^[6];

• Search DOE PAGES for author "Toney, Michael F."
• Search DOE PAGES for ORCID "0000-0002-7513-1166"

Hersam, Mark C.  ^[2];

• Search DOE PAGES for author "Hersam, Mark C."
• Search DOE PAGES for ORCID "0000-0003-4120-1426"

Elam, Jeffrey W.  ^[1]

• Search DOE PAGES for author "Elam, Jeffrey W."
• Search DOE PAGES for ORCID "0000-0002-5861-2996"

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+ Show Author Affiliations

1. Argonne National Lab. (ANL), Lemont, IL (United States)
2. Northwestern Univ., Evanston, IL (United States)
3. Argonne National Lab. (ANL), Lemont, IL (United States); Bruker Nano Surfaces, San Jose, CA (United States)
4. Univ. of Illinois at Chicago, Chicago, IL (United States)
5. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
6. SLAC National Accelerator Lab., Menlo Park, CA (United States)

Publication Date:

Mon Jul 09 00:00:00 EDT 2018

Research Org.:

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

Sponsoring Org.:

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

OSTI Identifier:

1476140

Alternate Identifier(s):

OSTI ID: 1493895

Grant/Contract Number:  

AC02-76SF00515; 1620901; AC02-06CH11357

Resource Type:

Accepted Manuscript

Journal Name:

ACS Applied Materials and Interfaces

Additional Journal Information:

Journal Volume: 10; Journal Issue: 32; Journal ID: ISSN 1944-8244

Publisher:

American Chemical Society (ACS)

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; atomic layer deposition; high shear modulus; lithium fluoride; lithium metal anode; new chemistry