Journal
ACS NANO
Volume 8, Issue 11, Pages 11560-11566Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nn504806h
Keywords
conversion/deconversion reaction; lithium-ion battery; in situ high-resolution electron microscopy; metal oxide electrode; electron diffraction
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Funding
- Center for Electrochemical Energy Science, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences
- NUANCE Center new initiatives
- MRSEC program at the Materials Research Center of the National Science Foundation [NSF DMR-1121262]
- Nanoscale Science and Engineering Center of the National Science Foundation [EEC-0118025/003]
- State of Illinois
- Northwestern University
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Electrode materials based on conversion reactions with lithium ions have shown much higher energy density than those based on intercalation reactions. Here, nanocubes of a typical metal oxide (Co3O4) were grown on few-layer graphene, and their electrochemical lithiation and delithiation were investigated at atomic resolution by in situ transmission electron microscopy to reveal the mechanism of the reversible conversion reaction. During lithiation, a lithium-inserted Co3O4 phase and a phase consisting of nanosized Co-Li-O clusters are identified as the intermediate products prior to the subsequent formation of Li2O crystals. In delithiation, the reduced metal nanoparticles form a network and breakdown into even smaller clusters that act as catalysts to prompt reduction of Li2O, and CoO nanoparticles are identified as the product of the deconversion reaction. Such direct real-space, real-time atomic-scale observations shed light on the phenomena and mechanisms in reaction-based electrochemical energy conversion and provide impetus for further development in electrochemical charge storage devices.
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