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Title: In situ quantification of interphasial chemistry in Li-ion battery

Journal Article · · Nature Nanotechnology
 [1];  [2];  [3];  [2];  [2];  [2];  [2];  [3]; ORCiD logo [3];  [4];  [5];  [2]
  1. Peking Univ., Shenzhen (China); Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Peking Univ., Shenzhen (China)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States); Stanford Univ., Stanford, CA (United States)
  5. US Army Research Lab., Adelphi, MD (United States)
+ Show Author Affiliations

The solid-electrolyte-interphase (SEI) is probably the least understood component in Li-ion batteries. Considerable effort has been put in the understanding of its formation and electrochemistry under realistic battery conditions, but mechanistic insights have been inferred mostly indirectly. Here we show the formation of the SEI between a graphite anode and a carbonate electrolyte using combined atomic scale microscopy and in-situ and operando techniques. In particular, we weigh the graphitic anode during its initial lithiation process with electrochemical quartz crystal microbalance, which unequivocally identifies lithium fluoride (LiF) and lithium alkylcarbonates as the main chemical components at different potentials. In-situ gas analysis confirmed the preferential reduction of cyclic over acyclic carbonate molecules, making its reduction product the major component in SEI. We find that SEI formation starts at graphite edge-sites with dimerization of solvated Li+-intercalation between graphite-layers. As a result, we also show that this lithium salt, at least in its nascent form, is re-oxidizable, despite the general belief that an SEI is electrochemically inert and its formation irreversible.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1493749
Journal Information:
Nature Nanotechnology, Vol. 14, Issue 1; ISSN 1748-3387
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (17)

Electrode Engineering by Atomic Layer Deposition for Sodium‐Ion Batteries: From Traditional to Advanced Batteries journal December 2019
Review of Recent Development of In Situ/Operando Characterization Techniques for Lithium Battery Research journal May 2019
In Operando Probing of Lithium‐Ion Storage on Single‐Layer Graphene journal March 2019
4.5 V High‐Voltage Rechargeable Batteries Enabled by the Reduction of Polarization on the Lithium Metal Anode journal August 2019
4.5 V High‐Voltage Rechargeable Batteries Enabled by the Reduction of Polarization on the Lithium Metal Anode journal October 2019
Plasma‐Enabled Ternary SnO 2 @Sn/Nitrogen‐Doped Graphene Aerogel Anode for Sodium‐Ion Batteries journal March 2020
Flexible Membrane Consisting of MoP Ultrafine Nanoparticles Highly Distributed Inside N and P Codoped Carbon Nanofibers as High‐Performance Anode for Potassium‐Ion Batteries journal December 2019
Deciphering the Interface of a High‐Voltage (5 V‐Class) Li‐Ion Battery Containing Additive‐Assisted Sulfolane‐Based Electrolyte journal September 2019
Microtubular carbon fibers derived from bamboo and wood as sustainable anodes for lithium and sodium ion batteries journal June 2019
Ultra-thin solid electrolyte interphase evolution and wrinkling processes in molybdenum disulfide-based lithium-ion batteries journal July 2019
Correlation between manganese dissolution and dynamic phase stability in spinel-based lithium-ion battery journal October 2019
Real-time mass spectrometric characterization of the solid–electrolyte interphase of a lithium-ion battery journal January 2020
A novel aqueous sodium–manganese battery system for energy storage journal January 2019
The stability and reaction mechanism of a LiF/electrolyte interface: insight from density functional theory journal January 2020
Active formation of Li-ion batteries and its effect on cycle life journal August 2019
Electrochemical Kinetics of SEI Growth on Carbon Black: Part I. Experiments journal January 2019
Ultra-thin solid electrolyte interphase evolution and wrinkling processes in molybdenum disulfide-based lithium-ion batteries journal July 2019

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