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Title: Nanoscale Nucleation and Growth of Electrodeposited Lithium Metal

Abstract

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.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [2]
+ Show Author Affiliations
  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:
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
OSTI Identifier:
1353101
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal Issue: 2; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; anode-free; anode-less; copper; electrodeposition; Lithium metal anode; nucleation and growth

Citation Formats

Pei, Allen, Zheng, Guangyuan, Shi, Feifei, Li, Yuzhang, and Cui, Yi. Nanoscale Nucleation and Growth of Electrodeposited Lithium Metal. United States: N. p., 2017. Web. doi:10.1021/acs.nanolett.6b04755.
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Pei, Allen, Zheng, Guangyuan, Shi, Feifei, Li, Yuzhang, & Cui, Yi. Nanoscale Nucleation and Growth of Electrodeposited Lithium Metal. United States. https://doi.org/10.1021/acs.nanolett.6b04755
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Pei, Allen, Zheng, Guangyuan, Shi, Feifei, Li, Yuzhang, and Cui, Yi. Tue . "Nanoscale Nucleation and Growth of Electrodeposited Lithium Metal". United States. https://doi.org/10.1021/acs.nanolett.6b04755. https://www.osti.gov/servlets/purl/1353101.
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@article{osti_1353101,
title = {Nanoscale Nucleation and Growth of Electrodeposited Lithium Metal},
author = {Pei, Allen and Zheng, Guangyuan and Shi, Feifei and Li, Yuzhang and Cui, Yi},
abstractNote = {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.},
doi = {10.1021/acs.nanolett.6b04755},
journal = {Nano Letters},
number = 2,
volume = 17,
place = {United States},
year = {2017},
month = {1}
}
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https://doi.org/10.1021/acs.nanolett.6b04755
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    A substrate-influenced three-dimensional unoriented dispersion pathway for dendrite-free lithium metal anodes
    journal, January 2018

    • Hu, Mengfei; Yuan, Yuan; Guo, Man
    • Journal of Materials Chemistry A, Vol. 6, Issue 30
    • DOI: 10.1039/c8ta04343d

    3D lithiophilic–lithiophobic–lithiophilic dual-gradient porous skeleton for highly stable lithium metal anode
    journal, January 2020

    • Zheng, Hongfei; Zhang, Qingfei; Chen, Qiulin
    • Journal of Materials Chemistry A, Vol. 8, Issue 1
    • DOI: 10.1039/c9ta09505e

    A bidirectional growth mechanism for a stable lithium anode by a platinum nanolayer sputtered on a polypropylene separator
    journal, January 2018

    • Wen, Kaihua; Liu, Lili; Chen, Shimou
    • RSC Advances, Vol. 8, Issue 23
    • DOI: 10.1039/c8ra02140f

    Uniform lithium deposition on N-doped carbon-coated current collectors
    journal, January 2019

    • Zhang, Na; Yu, Seung-Ho; Abruña, Héctor D.
    • Chemical Communications, Vol. 55, Issue 68
    • DOI: 10.1039/c9cc04415a

    Suppressing Lithium Dendrite Growth via Sinusoidal Ripple Current Produced by Triboelectric Nanogenerators
    journal, April 2019

    • Zhang, Zailei; Wang, Zhong Lin; Lu, Xianmao
    • Advanced Energy Materials, Vol. 9, Issue 20
    • DOI: 10.1002/aenm.201900487

    3D Wettable Framework for Dendrite-Free Alkali Metal Anodes
    journal, May 2018

    • Zhang, Ying; Wang, Chengwei; Pastel, Glenn
    • Advanced Energy Materials, Vol. 8, Issue 18
    • DOI: 10.1002/aenm.201800635

    Enabling Stable Lithium Metal Anode through Electrochemical Kinetics Manipulation
    journal, September 2019

    • Han, Yehu; Jie, Yulin; Huang, Fanyang
    • Advanced Functional Materials, Vol. 29, Issue 46
    • DOI: 10.1002/adfm.201904629

    Dendrite-Free Metallic Lithium in Lithiophilic Carbonized Metal-Organic Frameworks
    journal, March 2018

    Key Aspects of Lithium Metal Anodes for Lithium Metal Batteries
    journal, March 2019

    Self-heating–induced healing of lithium dendrites
    journal, March 2018

    Reliable seawater battery anode: controlled sodium nucleation via deactivation of the current collector surface
    journal, January 2018

    • Kim, Do Hyeong; Choi, Hongkyw; Hwang, Dae Yeon
    • Journal of Materials Chemistry A, Vol. 6, Issue 40
    • DOI: 10.1039/c8ta07610c

    Operando monitoring the lithium spatial distribution of lithium metal anodes
    journal, June 2018

    Effect of Temperature on Li Electrodeposition Behavior in Room-Temperature Ionic Liquids Comprising Quaternary Ammonium Cation
    journal, January 2019

    • Sano, Hikaru; Kitta, Mitsunori; Shikano, Masahiro
    • Journal of The Electrochemical Society, Vol. 166, Issue 13
    • DOI: 10.1149/2.1051913jes

    Constructing Ionic Gradient and Lithiophilic Interphase for High‐Rate Li‐Metal Anode
    journal, October 2019

    First‐Principles Studies of Li Nucleation on Double‐Layered Defective Graphene
    journal, September 2018

    Achieving a stable Na metal anode with a 3D carbon fibre scaffold
    journal, January 2018

    • Zhang, Qiu; Lu, Yanying; Zhou, Meng
    • Inorganic Chemistry Frontiers, Vol. 5, Issue 4
    • DOI: 10.1039/c7qi00802c

    Understanding the molecular mechanism of pulse current charging for stable lithium-metal batteries
    journal, July 2017

    • Li, Qi; Tan, Shen; Li, Linlin
    • Science Advances, Vol. 3, Issue 7, Article No. e1701246
    • DOI: 10.1126/sciadv.1701246

    Lithiophilic NiO hexagonal plates decorated Ni collector guiding uniform lithium plating for stable lithium metal anode
    journal, January 2019

    • Lu, Weiyi; Wu, Chen; Wei, Weifeng
    • Journal of Materials Chemistry A, Vol. 7, Issue 42
    • DOI: 10.1039/c9ta09396f

    Reducing lithium deposition overpotential with silver nanocrystals anchored on graphene aerogel
    journal, January 2018

    • Wang, Xianshu; Pan, Zhenghui; Wu, Yang
    • Nanoscale, Vol. 10, Issue 35
    • DOI: 10.1039/c8nr04655g

    Stable Li Metal Anodes via Regulating Lithium Plating/Stripping in Vertically Aligned Microchannels
    journal, September 2017

    • Wang, Shu-Hua; Yin, Ya-Xia; Zuo, Tong-Tong
    • Advanced Materials, Vol. 29, Issue 40
    • DOI: 10.1002/adma.201703729

    Stable Nano‐Encapsulation of Lithium Through Seed‐Free Selective Deposition for High‐Performance Li Battery Anodes
    journal, January 2020

    Deterministic growth of a sodium metal anode on a pre-patterned current collector for highly rechargeable seawater batteries
    journal, January 2019

    • Jung, Jaeho; Hwang, Dae Yeon; Kristanto, Imanuel
    • Journal of Materials Chemistry A, Vol. 7, Issue 16
    • DOI: 10.1039/c9ta01718f

    Lithiophilicity chemistry of heteroatom-doped carbon to guide uniform lithium nucleation in lithium metal anodes
    journal, February 2019

    Suppression of dendritic lithium growth in lithium metal-based batteries
    journal, January 2018

    • Li, Linlin; Li, Siyuan; Lu, Yingying
    • Chemical Communications, Vol. 54, Issue 50
    • DOI: 10.1039/c8cc02280a

    Reducing the Interfacial Resistance in All‐Solid‐State Lithium Batteries Based on Oxide Ceramic Electrolytes
    journal, April 2019

    Predicting Calendar Aging in Lithium Metal Secondary Batteries: The Impacts of Solid Electrolyte Interphase Composition and Stability
    journal, August 2018

    • Wood, Sean M.; Fang, Chengcheng; Dufek, Eric J.
    • Advanced Energy Materials, Vol. 8, Issue 26
    • DOI: 10.1002/aenm.201801427

    Temperature‐dependent Nucleation and Growth of Dendrite‐Free Lithium Metal Anodes
    journal, July 2019

    Electromigration in Lithium Whisker Formation Plays Insignificant Role during Electroplating
    journal, January 2019

    • Rulev, Alexey A.; Sergeev, Artem V.; Yashina, Lada V.
    • ChemElectroChem, Vol. 6, Issue 5
    • DOI: 10.1002/celc.201801652

    Effect of glyphosate on X-ray diffraction of copper films prepared by electrochemical deposition
    journal, January 2019

    • Zhang, Gaomin; Xu, Bin; Chong, Hui
    • RSC Advances, Vol. 9, Issue 25
    • DOI: 10.1039/c9ra01385g

    The Three‐Dimensional Dendrite‐Free Zinc Anode on a Copper Mesh with a Zinc‐Oriented Polyacrylamide Electrolyte Additive
    journal, September 2019

    Rethinking sodium-ion anodes as nucleation layers for anode-free batteries
    journal, January 2018

    • Cohn, Adam P.; Metke, Thomas; Donohue, Jennifer
    • Journal of Materials Chemistry A, Vol. 6, Issue 46
    • DOI: 10.1039/c8ta05911j

    Long Cycle Life Lithium Metal Batteries Enabled with Upright Lithium Anode
    journal, February 2019

    • Chen, Yuqing; Yue, Meng; Liu, Cuilian
    • Advanced Functional Materials, Vol. 29, Issue 15
    • DOI: 10.1002/adfm.201806752

    An Aggregate Cluster-Dispersed Electrolyte Guides the Uniform Nucleation and Growth of Lithium at Lithium Metal Anodes
    journal, November 2018

    A facile annealing strategy for achieving in situ controllable Cu 2 O nanoparticle decorated copper foil as a current collector for stable lithium metal anodes
    journal, January 2018

    • Zhang, Qi; Luan, Jingyi; Tang, Yougen
    • Journal of Materials Chemistry A, Vol. 6, Issue 38
    • DOI: 10.1039/c8ta07612j

    The Challenge of Lithium Metal Anodes for Practical Applications
    journal, April 2019

    Electrotunable liquid sulfur microdroplets
    journal, January 2020

    A collaborative strategy for stable lithium metal anodes by using three-dimensional nitrogen-doped graphene foams
    journal, January 2018

    Vertically Aligned Lithiophilic CuO Nanosheets on a Cu Collector to Stabilize Lithium Deposition for Lithium Metal Batteries
    journal, April 2018

    • Zhang, Chen; Lv, Wei; Zhou, Guangmin
    • Advanced Energy Materials, Vol. 8, Issue 21
    • DOI: 10.1002/aenm.201703404

    Bottom-top channeling Li nucleation and growth by a gradient lithiophilic 3D conductive host for highly stable Li-metal anodes
    journal, January 2020

    • Yan, Xiaolin; Zhang, Qingfei; Xu, Wanjie
    • Journal of Materials Chemistry A, Vol. 8, Issue 4
    • DOI: 10.1039/c9ta11311h

    Spatial separation of lithiophilic surface and superior conductivity for advanced Li metal anode: the case of acetylene black and N-doped carbon spheres
    journal, January 2019

    • Liang, Feng; Lin, Liangdong; Feng, Zhenyu
    • Journal of Materials Chemistry A, Vol. 7, Issue 15
    • DOI: 10.1039/c9ta00742c

    Ultrathin Bilayer of Graphite/SiO 2 as Solid Interface for Reviving Li Metal Anode
    journal, August 2019

    • Pathak, Rajesh; Chen, Ke; Gurung, Ashim
    • Advanced Energy Materials, Vol. 9, Issue 36
    • DOI: 10.1002/aenm.201901486

    Pristine or Highly Defective? Understanding the Role of Graphene Structure for Stable Lithium Metal Plating
    journal, November 2018

    Control of the adhesion strength between nickel replica and copper mold by electrochemical nucleation of lead
    journal, August 2019

    Electrochemomechanics of lithium dendrite growth
    journal, January 2019

    • Jana, Aniruddha; Woo, Sang Inn; Vikrant, K. S. N.
    • Energy & Environmental Science, Vol. 12, Issue 12
    • DOI: 10.1039/c9ee01864f

    Controlling Nucleation in Lithium Metal Anodes
    journal, July 2018

    Towards high rate Li metal anodes: enhanced performance at high current density in a superconcentrated ionic liquid
    journal, January 2020

    • Periyapperuma, Kalani; Arca, Elisabetta; Harvey, Steve
    • Journal of Materials Chemistry A, Vol. 8, Issue 7
    • DOI: 10.1039/c9ta12004a

    Printable Fabrication of Nanocoral-Structured Electrodes for High-Performance Flexible and Planar Supercapacitor with Artistic Design
    journal, October 2017

    A Material Perspective of Rechargeable Metallic Lithium Anodes
    journal, February 2018

    Stable Lithium Electrodeposition at Ultra-High Current Densities Enabled by 3D PMF/Li Composite Anode
    journal, February 2018

    • Fan, Lei; Zhuang, Houlong L.; Zhang, Weidong
    • Advanced Energy Materials, Vol. 8, Issue 15
    • DOI: 10.1002/aenm.201703360

    Magnetic Field–Suppressed Lithium Dendrite Growth for Stable Lithium‐Metal Batteries
    journal, April 2019

    • Shen, Kang; Wang, Zeng; Bi, Xuanxuan
    • Advanced Energy Materials, Vol. 9, Issue 20
    • DOI: 10.1002/aenm.201900260

    Lithiophilic Sites in Doped Graphene Guide Uniform Lithium Nucleation for Dendrite-Free Lithium Metal Anodes
    journal, May 2017

    Enhanced Stability of Lithium Metal Anode by using a 3D Porous Nickel Substrate
    journal, February 2018

    Large‐Scale Modification of Commercial Copper Foil with Lithiophilic Metal Layer for Li Metal Battery
    journal, January 2020

    Fast galvanic lithium corrosion involving a Kirkendall-type mechanism
    journal, January 2019

    Ladderlike carbon nanoarrays on 3D conducting skeletons enable uniform lithium nucleation for stable lithium metal anodes
    journal, January 2018

    • Liu, Lin; Yin, Ya-Xia; Li, Jin-Yi
    • Chemical Communications, Vol. 54, Issue 42
    • DOI: 10.1039/c8cc02672f

    Nanoscale in situ detection of nucleation and growth of Li electrodeposition at various current densities
    journal, January 2018

    • Jung, Haesung; Lee, Byeongdu; Lengyel, Miklos
    • Journal of Materials Chemistry A, Vol. 6, Issue 11
    • DOI: 10.1039/c8ta00343b

    Depressing the irreversible reactions on a three-dimensional interface towards a high-areal capacity lithium metal anode
    journal, January 2019

    • Deng, Wei; Liang, Shanshan; Zhou, Xufeng
    • Journal of Materials Chemistry A, Vol. 7, Issue 11
    • DOI: 10.1039/c9ta00143c

    The effect of local lithium surface chemistry and topography on solid electrolyte interphase composition and dendrite nucleation
    journal, January 2019

    • Meyerson, Melissa L.; Sheavly, Jonathan K.; Dolocan, Andrei
    • Journal of Materials Chemistry A, Vol. 7, Issue 24
    • DOI: 10.1039/c9ta03371h

    Uniform Li deposition by regulating the initial nucleation barrier via a simple liquid-metal coating for a dendrite-free Li–metal anode
    journal, January 2019

    • Wei, Chuanliang; Fei, Huifang; An, Yongling
    • Journal of Materials Chemistry A, Vol. 7, Issue 32
    • DOI: 10.1039/c9ta06663b

    Stabilizing a sodium-metal battery with the synergy effects of a sodiophilic matrix and fluorine-rich interface
    journal, January 2019

    • Wang, Qidi; Zhao, Chenglong; Lv, Xiaohui
    • Journal of Materials Chemistry A, Vol. 7, Issue 43
    • DOI: 10.1039/c9ta06877e

    Nitrogen-doped graphdiyne nanowall stabilized dendrite-free lithium metal anodes
    journal, January 2019

    • Jiang, Tao; Chen, Ke; Wang, Jingjing
    • Journal of Materials Chemistry A, Vol. 7, Issue 48
    • DOI: 10.1039/c9ta09551a

    Columnar Lithium Metal Anodes
    journal, September 2017

    Rethinking How External Pressure Can Suppress Dendrites in Lithium Metal Batteries
    journal, January 2019

    • Zhang, Xin; Wang, Q. Jane; Harrison, Katharine L.
    • Journal of The Electrochemical Society, Vol. 166, Issue 15
    • DOI: 10.1149/2.0701914jes

    Favorable Lithium Nucleation on Lithiophilic Framework Porphyrin for Dendrite-Free Lithium Metal Anodes
    journal, January 2019

    Synergistic Effect of 3D Current Collectors and ALD Surface Modification for High Coulombic Efficiency Lithium Metal Anodes
    journal, September 2019

    • Chen, Kuan-Hung; Sanchez, Adrian J.; Kazyak, Eric
    • ECS Meeting Abstracts, Vol. MA2019-02, Issue 6
    • DOI: 10.1149/ma2019-02/6/527
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