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Distinct charge dynamics in battery electrodes revealed by in situ and operando soft X-ray spectroscopy

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms3568· OSTI ID:1623927
 [1];  [2];  [2];  [2];  [3];  [4];  [4]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Inst. of Microsystem and Information Technology. State Key Lab. of Functional Materials for Informatics; DOE/OSTI
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Environmental Energy Technologies Division
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Inst. of Microsystem and Information Technology. State Key Lab. of Functional Materials for Informatics
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Developing high-performance batteries relies on material breakthroughs. During the past few years, various in situ characterization tools have been developed and have become indispensible in studying and the eventual optimization of battery materials. However, soft X-ray spectroscopy, one of the most sensitive probes of electronic states, has been mainly limited to ex situ experiments for battery research. Here we achieve in situ and operando soft X-ray absorption spectroscopy of lithium-ion battery cathodes. Taking advantage of the elemental, chemical and surface sensitivities of soft X-rays, we discover distinct lithium-ion and electron dynamics in Li(Co1/3Ni1/3Mn1/3)O2 and LiFePO4 cathodes in polymer electrolytes. The contrast between the two systems and the relaxation effect in LiFePO4 is attributed to a phase transformation mechanism, and the mesoscale morphology and charge conductivity of the electrodes. These discoveries demonstrate feasibility and power of in situ soft X-ray spectroscopy for studying integrated and dynamic effects in batteries.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1623927
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 4; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (40)

Quantifying Bulk Electrode Strain and Material Displacement within Lithium Batteries via High-Speed Operando Tomography and Digital Volume Correlation journal December 2015
Following lithiation fronts in paramagnetic electrodes with in situ magnetic resonance spectroscopic imaging journal November 2016
Coupling between oxygen redox and cation migration explains unusual electrochemistry in lithium-rich layered oxides journal December 2017
Elucidating anionic oxygen activity in lithium-rich layered oxides journal March 2018
Operando X-Ray Spectroscopic Techniques: A Focus on Hydrogen and Oxygen Evolution Reactions journal January 2020
Atomic Insights into the Enhanced Surface Stability in High Voltage Cathode Materials by Ultrathin Coating journal January 2017
Recent Progress on Synchrotron-Based In-Situ Soft X-ray Spectroscopy for Energy Materials journal May 2014
Atomic-Scale Structure Evolution in a Quasi-Equilibrated Electrochemical Process of Electrode Materials for Rechargeable Batteries journal February 2015
Persistent State-of-Charge Heterogeneity in Relaxed, Partially Charged Li 1− x Ni 1/3 Co 1/3 Mn 1/3 O 2 Secondary Particles journal May 2016
Anionic Redox in Rechargeable Lithium Batteries journal June 2017
Review of Recent Development of In Situ/Operando Characterization Techniques for Lithium Battery Research journal May 2019
In Situ Formation of a Cathode-Electrolyte Interface with Enhanced Stability by Titanium Substitution for High Voltage Spinel Lithium-Ion Batteries journal May 2015
Trimetallic Sulfide Mesoporous Nanospheres as Superior Electrocatalysts for Rechargeable Zn-Air Batteries journal October 2018
Quantification of Heterogeneous Degradation in Li‐Ion Batteries journal May 2019
Conductive Copper Niobate: Superior Li + ‐Storage Capability and Novel Li + ‐Transport Mechanism journal August 2019
Towards a Safe Lithium-Sulfur Battery with a Flame-Inhibiting Electrolyte and a Sulfur-Based Composite Cathode journal July 2014
Towards a Safe Lithium-Sulfur Battery with a Flame-Inhibiting Electrolyte and a Sulfur-Based Composite Cathode journal July 2014
Operando Observation of Formation and Annihilation of Inhomogeneous Reaction Distribution in a Composite Electrode for Lithium‐Ion Batteries journal April 2019
Synchrotron-Based X-ray Absorption Fine Structures, X-ray Diffraction, and X-ray Microscopy Techniques Applied in the Study of Lithium Secondary Batteries journal April 2018
In Situ Probing Multiple-Scale Structures of Energy Materials for Li-Ion Batteries journal May 2019
The Advances of Metal Sulfides and In Situ Characterization Methods beyond Li Ion Batteries: Sodium, Potassium, and Aluminum Ion Batteries journal November 2019
DFT study of nano zinc/copper voltaic cells journal March 2018
Theory-driven design of high-valence metal sites for water oxidation confirmed using in situ soft X-ray absorption journal November 2017
In operando tracking phase transformation evolution of lithium iron phosphate with hard X-ray microscopy journal August 2014
State-of-the-art characterization techniques for advanced lithium-ion batteries journal March 2017
Microscopic photoelectron analysis of single crystalline LiCoO2 particles during the charge-discharge in an all solid-state lithium ion battery journal August 2019
Electronic structure variation of the surface and bulk of a LiNi 0.5 Mn 1.5 O 4 cathode as a function of state of charge: X-ray absorption spectroscopic study journal January 2014
Profiling the nanoscale gradient in stoichiometric layered cathode particles for lithium-ion batteries journal January 2014
Influence of synthesis conditions on the surface passivation and electrochemical behavior of layered cathode materials journal January 2014
Highly wettable and metallic NiFe-phosphate/phosphide catalyst synthesized by plasma for highly efficient oxygen evolution reaction journal January 2018
Single-crystal based studies for correlating the properties and high-voltage performance of Li[Ni x Mn y Co 1−x−y ]O 2 cathodes journal January 2019
Quantitative in situ 13 C NMR studies of the electro-catalytic oxidation of ethanol journal January 2019
Modular soft x-ray spectrometer for applications in energy sciences and quantum materials journal January 2017
The development of 2D materials for electrochemical energy applications: A mechanistic approach journal March 2019
Quantitative probe of the transition metal redox in battery electrodes through soft x-ray absorption spectroscopy journal September 2016
Using in situ and operando methods to characterize phase changes in charged lithium nickel cobalt aluminum oxide cathode materials journal January 2020
Theory of L -edge spectroscopy of strongly correlated systems journal December 2017
In situ visualization of Li/Ag2VP2O8 batteries revealing rate-dependent discharge mechanism journal January 2015
Improving the Rate Capability of LiFePO 4 Electrode by Controlling Particle Size Distribution journal January 2019
X-ray Absorption Spectroscopy Characterization of a Li/S Cell journal January 2016

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