Observation and Quantification of Nanoscale Processes in Lithium Batteries by Operando Electrochemical (S)TEM

Journal Article · Wed Mar 11 04:00:00 EDT 2015 · Nano Letters, 15(3):2168-2176

DOI:https://doi.org/10.1021/acs.nanolett.5b00175· OSTI ID:1184939

Mehdi, Beata L.; Qian, Jiangfeng; Nasybulin, Eduard; Park, Chiwoo; Welch, David A.; Faller, Roland; Mehta, Hardeep S.; Henderson, Wesley A.; Xu, Wu; Wang, Chong M.; Evans, James E.; Liu, Jun; Zhang, Jiguang; Mueller, Karl T.; Browning, Nigel D.

An operando electrochemical stage for the transmission electron microscope has been configured to form a “Li battery” that is used to quantify the electrochemical processes that occur at the anode during charge/discharge cycling. Of particular importance for these observations is the identification of an image contrast reversal that originates from solid Li being less dense than the surrounding liquid electrolyte and electrode surface. This contrast allows Li to be identified from Li containing compounds that make up the solid-electrolyte interphase (SEI) layer. By correlating images showing the sequence of Li electrodeposition and the evolution of the SEI layer with simultaneously acquired and calibrated cyclic voltammograms (CV), electrodeposition and electrolyte breakdown processes can be quantified directly on the nanoscale. This approach opens up intriguing new possibilities to rapidly visualize and test the electrochemical performance of a wide range of electrode/electrolyte combinations for next generation battery systems.

• Research Organization: Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
• Sponsoring Organization: USDOE
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 1184939
• Report Number(s): PNNL-SA-107504; 48681; KC0208010
• Journal Information: Nano Letters, 15(3):2168-2176, Journal Name: Nano Letters, 15(3):2168-2176
• Country of Publication: United States
• Language: English

Related Subjects

Environmental Molecular Sciences Laboratory
Li Batteries
Li dendrite formation
Li deposition/dissolution
Operando Scanning Transmission Electron Microscopy
SEI Layer
in-situ electrochemical liquid cell