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Title: Formation and Inhibition of Metallic Lithium Microstructures in Lithium Batteries Driven by Chemical Crossover

The formation of metallic lithium microstructures in the form of dendrites or mosses at the surface of anode electrodes (e.g., lithium metal, graphite, and silicon) leads to rapid capacity fade and poses grave safety risks in rechargeable lithium batteries. In this work, we present here a direct, relative quantitative analysis of lithium deposition on graphite anodes in pouch cells under normal operating conditions, paired with a model cathode material, the layered nickel-rich oxide LiNi 0.61Co 0.12Mn 0.27O 2, over the course of 3000 charge-discharge cycles. Secondary-ion mass spectrometry chemically dissects the solid-electrolyte interphase (SEI) on extensively cycled graphite with virtually atomic depth resolution and reveals substantial growth of Li-metal deposits. With the absence of apparent kinetic (e.g., fast charging) or stoichiometric restraints (e.g., overcharge) during cycling, we show lithium deposition on graphite is triggered by certain transition-metal ions (manganese in particular) dissolved from the cathode in a disrupted SEI. This insidious effect is found to initiate at a very early stage of cell operation (<200 cycles) and can be effectively inhibited by substituting a small amount of aluminum (~1 mol %) in the cathode, resulting in much reduced transition-metal dissolution and drastically improved cyclability. In conclusion, our results may alsomore » be applicable to studying the unstable electrodeposition of lithium on other substrates, including Li metal.« less
 [1] ;  [2] ; ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [1]
  1. Univ. of Texas, Austin, TX (United States). Materials Science and Engineering Program and Texas Materials Institute
  2. Hanyang University, Seoul (Korea, Republic of). Department of Energy Engineering
Publication Date:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 11; Journal Issue: 6; Journal ID: ISSN 1936-0851
American Chemical Society (ACS)
Research Org:
Univ. of Texas, Austin, TX (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Country of Publication:
United States
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; carbon anodes; lithium deposition; lithium-ion batteries; nickel-rich layered oxides; secondary-ion mass spectrometry; transition-metal dissolution
OSTI Identifier: