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Title: Nanoscale Nucleation and Growth of Electrodeposited Lithium Metal

Lithium metal has re-emerged as an exciting anode for high energy lithium-ion batteries due to its high specific capacity of 3860 mAh g -1 and lowest electrochemical potential of all known materials. However, lithium has been plagued by the issues of dendrite formation, high chemical reactivity with electrolyte, and infinite relative volume expansion during plating and stripping, which present safety hazards and low cycling efficiency in batteries with lithium metal electrodes. There have been a lot of recent studies on Li metal although little work has focused on the initial nucleation and growth behavior of Li metal, neglecting a critical fundamental scientific foundation of Li plating. Here, we study experimentally the morphology of lithium in the early stages of nucleation and growth on planar copper electrodes in liquid organic electrolyte. We elucidate the dependence of lithium nuclei size, shape, and areal density on current rate, consistent with classical nucleation and growth theory. We found that the nuclei size is proportional to the inverse of overpotential and the number density of nuclei is proportional to the cubic power of overpotential. Finally, based on this understanding, we propose a strategy to increase the uniformity of electrodeposited lithium on the electrode surface.
ORCiD logo [1] ;  [1] ;  [1] ;  [1] ;  [2]
  1. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
  2. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
Publication Date:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal Issue: 2; Journal ID: ISSN 1530-6984
American Chemical Society
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOD
Country of Publication:
United States
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; anode-free; anode-less; copper; electrodeposition; Lithium metal anode; nucleation and growth
OSTI Identifier: