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Title: Dendrites and Pits: Untangling the Complex Behavior of Lithium Metal Anodes through Operando Video Microscopy

Enabling ultra-high energy density rechargeable Li batteries would have widespread impact on society. But, the critical challenges of Li metal anodes (most notably cycle life and safety) remain unsolved. This is attributed to the evolution of Li metal morphology during cycling, which leads to dendrite growth and surface pitting. Herein, we present a comprehensive understanding of the voltage variations observed during Li metal cycling, which is directly correlated to morphology evolution through the use of operando video microscopy. A custom-designed visualization cell was developed to enable operando synchronized observation of Li metal electrode morphology and electrochemical behavior during cycling. A mechanistic understanding of the complex behavior of these electrodes is gained through correlation with continuum-scale modeling, which provides insight into the dominant surface kinetics. Our work provides a detailed explanation of (1) when dendrite nucleation occurs, (2) how those dendrites evolve as a function of time, (3) when surface pitting occurs during Li electrodissolution, (4) kinetic parameters that dictate overpotential as the electrode morphology evolves, and (5) how this understanding can be applied to evaluate electrode performance in a variety of electrolytes. Our results provide detailed insight into the interplay between morphology and the dominant electrochemical processes occurring on themore » Li electrode surface through an improved understanding of changes in cell voltage, which represents a powerful new platform for analysis.« less
Authors:
 [1] ;  [2] ;  [3] ;  [2] ;  [4] ;  [5] ;  [1]
  1. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Mechanical Engineering and Joint Center for Energy Storage Research
  2. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Mechanical Engineering
  3. Univ. of Michigan, Ann Arbor, MI (United States). Joint Center for Energy Storage Research
  4. Univ. of Michigan, Ann Arbor, MI (United States). Joint Center for Energy Storage Research; Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy and Environmental Directorate
  5. Univ. of Michigan, Ann Arbor, MI (United States). Joint Center for Energy Storage Research and Dept. of Materials Science and Engineering
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Published Article
Journal Name:
ACS Central Science
Additional Journal Information:
Journal Volume: 2; Journal Issue: 11; Journal ID: ISSN 2374-7943
Publisher:
American Chemical Society (ACS)
Research Org:
Univ. of Michigan, Ann Arbor, MI (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE
OSTI Identifier:
1328970
Alternate Identifier(s):
OSTI ID: 1334179