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Title: Operando and three-dimensional visualization of anion depletion and lithium growth by stimulated Raman scattering microscopy

Journal Article · · Nature Communications

Visualization of ion transport in electrolytes provides fundamental understandings of electrolyte dynamics and electrolyte-electrode interactions. However, this is challenging because existing techniques are hard to capture low ionic concentrations and fast electrolyte dynamics. Here we show that stimulated Raman scattering microscopy offers required resolutions to address a long-lasting question: how does the lithium-ion concentration correlate to uneven lithium deposition? In this study, anions are used to represent lithium ions since their concentrations should not deviate for more than 0.1 mM, even near nanoelectrodes. A three-stage lithium deposition process is uncovered, corresponding to no depletion, partial depletion, and full depletion of lithium ions. Further analysis reveals a feedback mechanism between the lithium dendrite growth and heterogeneity of local ionic concentration, which can be suppressed by artificial solid electrolyte interphase. This report shows that stimulated Raman scattering microscopy is a powerful tool for the materials and energy field.

Research Organization:
Michigan State Univ., East Lansing, MI (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Grant/Contract Number:
EE0007803
OSTI ID:
1513262
Journal Information:
Nature Communications, Vol. 9, Issue 1; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 123 works
Citation information provided by
Web of Science

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The Formation Mechanism of Fluorescent Metal Complexes at the Li x Ni 0.5 Mn 1.5 O 4−δ /Carbonate Ester Electrolyte Interface journal March 2015
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Issues and challenges facing rechargeable lithium batteries journal November 2001
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Nanoionics: ion transport and electrochemical storage in confined systems journal November 2005
7Li MRI of Li batteries reveals location of microstructural lithium journal February 2012
Reviving the lithium metal anode for high-energy batteries journal March 2017
Effective NaCl and dye rejection of hybrid graphene oxide/graphene layered membranes journal August 2017
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Nanodiamonds suppress the growth of lithium dendrites journal August 2017
Non-encapsulation approach for high-performance Li–S batteries through controlled nucleation and growth journal September 2017
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Raman Spectroelectrochemistry of a Lithium/Polymer Electrolyte Symmetric Cell journal January 1998
Effect of Additives on Lithium Cycling Efficiency journal January 1994
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Cited By (19)

Pseudocapacitance Induced Uniform Plating/Stripping of Li Metal Anode in Vertical Graphene Nanowalls journal October 2018
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Interlayered Dendrite‐Free Lithium Plating for High‐Performance Lithium‐Metal Batteries journal May 2019
Magnetic Field–Suppressed Lithium Dendrite Growth for Stable Lithium‐Metal Batteries journal April 2019
In Situ Conversion of Cu 3 P Nanowires to Mixed Ion/Electron‐Conducting Skeleton for Homogeneous Lithium Deposition journal November 2019
Fluorescence Probing of Active Lithium Distribution in Lithium Metal Anodes journal April 2019
Fluorescence Probing of Active Lithium Distribution in Lithium Metal Anodes journal April 2019
Recent Progress in Polysulfide Redox‐Flow Batteries journal June 2019
New Insights into Nail Penetration of Li‐Ion Batteries: Effects of Heterogeneous Contact Resistance journal July 2019
Rapid, 3D Chemical Profiling of Individual Atmospheric Aerosols with Stimulated Raman Scattering Microscopy journal December 2019
Rational design of spontaneous reactions for protecting porous lithium electrodes in lithium–sulfur batteries journal July 2019
3D hollow reduced graphene oxide foam as a stable host for high-capacity lithium metal anodes journal January 2019
Fabricating ferromagnetic MoS 2 -based composite exposed to simulated sunlight for sodium storage journal January 2019
Towards high energy density lithium battery anodes: silicon and lithium journal January 2019
Probe design for super-multiplexed vibrational imaging journal April 2019
Synergistic Effects of Salt Concentration and Working Temperature towards Dendrite-Free Lithium Deposition journal October 2019
Rational design of spontaneous reactions for protecting porous lithium electrodes in lithium–sulfur batteries journal July 2019
Synergistic Effects of Salt Concentration and Working Temperature towards Dendrite-Free Lithium Deposition journal October 2019

Figures / Tables (6)