4.8 Article

Revealing Nanoscale Passivation and Corrosion Mechanisms of Reactive Battery Materials in Gas Environments

Journal

NANO LETTERS
Volume 17, Issue 8, Pages 5171-5178

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.7b02630

Keywords

In situ TEM; lithium metal battery; environmental TEM; passivation; corrosion

Funding

  1. National Science Foundation Graduate Research Fellowship Program (NSF GRFP)
  2. U.S. Department of Defense through the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program
  3. Stanford University through the Stanford Graduate Fellowship (SGF) Program
  4. German Research Foundation (DFG) [BU 2875/2-1]

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Lithium (Li) metal is a high-capacity anode material (3860 mAh g(-1)) that can enable high-energy batteries for electric vehicles and grid-storage applications. However, Li metal is highly reactive and repeatedly consumed when exposed to liquid electrolyte (during battery operation) or the ambient environment (throughout battery manufacturing). Studying these corrosion reactions on the nanoscale is especially difficult due to the high chemical reactivity of both Li metal and its surface corrosion films. Here, we directly generate pure Li metal inside an environmental transmission electron microscope (TEM), revealing the nanoscale passivation and corrosion process of Li metal in oxygen (O-2), nitrogen (N-2), and water vapor (H2O). We find that while dry O-2 and N-2 (99.9999 vol %) form uniform passivation layers on Li, trace water vapor (similar to 1 mol %) disrupts this passivation and forms a porous film on Li metal that allows gas to penetrate and continuously react with Li. To exploit the self-passivating behavior of Li in dry conditions, we introduce a simple dry-N-2 pretreatment of Li metal to form a protective layer of Li nitride prior to battery assembly. The fast ionic conductivity and stable interface of Li nitride results in improved battery performance with dendrite-free cycling and low voltage hysteresis. Our work reveals the detailed process of Li metal passivation/corrosion and demonstrates how this mechanistic insight can guide engineering solutions for Li metal batteries.

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