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

Wood, Kevin N.; Kazyak, Eric; Chadwick, Alexander F.; Chen, Kuan-Hung; Zhang, Ji-Guang; Thornton, Katsuyo; Dasgupta, Neil P.

doi:10.1021/acscentsci.6b00260

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

Journal Article · Fri Oct 14 00:00:00 EDT 2016 · ACS Central Science

DOI:https://doi.org/10.1021/acscentsci.6b00260· OSTI ID:1328970

Wood, Kevin N. ^[1]; Kazyak, Eric ^[2]; Chadwick, Alexander F. ^[3]; Chen, Kuan-Hung ^[2]; Zhang, Ji-Guang ^[4]; Thornton, Katsuyo ^[3]; Dasgupta, Neil P. ^[1]

Department of Mechanical Engineering, University of Michigan, Ann Arbor, Michigan 48109, United States, Joint Center for Energy Storage Research, University of Michigan, Ann Arbor, Michigan 48109, United States
Department of Mechanical Engineering, University of Michigan, Ann Arbor, Michigan 48109, United States
Joint Center for Energy Storage Research, University of Michigan, Ann Arbor, Michigan 48109, United States, Department of Materials Science and Engineering, University of Michigan, Ann Arbor, Michigan 48109, United States
Joint Center for Energy Storage Research, University of Michigan, Ann Arbor, Michigan 48109, United States, Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States

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 the Li electrode surface through an improved understanding of changes in cell voltage, which represents a powerful new platform for analysis.

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Research Organization:: Univ. of Michigan, Ann Arbor, MI (United States)

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

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1328970

Alternate ID(s):: OSTI ID: 1334179

Journal Information:: ACS Central Science, Journal Name: ACS Central Science Vol. 2 Journal Issue: 11; ISSN 2374-7943

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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