Document Detail

Nanoscale Imaging of Lithium Ion Distribution During In Situ Operation of Battery Electrode and Electrolyte.
MedLine Citation:
PMID:  24548177     Owner:  NLM     Status:  Publisher    
A major challenge in the development of new battery materials is understanding their fundamental mechanisms of operation and degradation. Their microscopically inhomogeneous nature calls for characterization tools that provide operando and localized information from individual grains and particles. Here we describe an approach that enables imaging of the nanoscale distribution of ions during electrochemical charging of a battery in a transmission electron microscope liquid flow cell. We use valence energy-loss spectroscopy to track both solvated and intercalated ions, with electronic structure fingerprints of the solvated ions identified using an ab initio non-linear response theory. Equipped with the new electrochemical cell holder, nanoscale spectroscopy and theory, we have been able to determine the lithiation state of a LiFePO4 electrode and surrounding aqueous electrolyte in real time with nanoscale resolution during electrochemical charge and discharge. We follow lithium transfer between electrode and electrolyte and image charging dynamics in the cathode. We observe competing delithiation mechanisms such as core-shell and anisotropic growth occurring in parallel for different particles under the same conditions. This technique represents a general approach for the operando nanoscale imaging of electrochemically active ions in the electrode and electrolyte in a wide range of electrical energy storage systems.
Megan E Holtz; Yingchao Yu; Deniz Gunceler; Jie Gao; Ravishankar Sundararaman; Kathleen A Schwarz; Tomás A Arias; Héctor D Abruña; David A Muller
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Publication Detail:
Type:  JOURNAL ARTICLE     Date:  2014-2-18
Journal Detail:
Title:  Nano letters     Volume:  -     ISSN:  1530-6992     ISO Abbreviation:  Nano Lett.     Publication Date:  2014 Feb 
Date Detail:
Created Date:  2014-2-19     Completed Date:  -     Revised Date:  -    
Medline Journal Info:
Nlm Unique ID:  101088070     Medline TA:  Nano Lett     Country:  -    
Other Details:
Languages:  ENG     Pagination:  -     Citation Subset:  -    
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