期刊
NANO LETTERS
卷 14, 期 3, 页码 1453-1459出版社
AMER CHEMICAL SOC
DOI: 10.1021/nl404577c
关键词
operando; in situ; TEM; Li-ion battery; LiFePO4; EFTEM
类别
资金
- National Science Foundation Materials Research Science and Engineering Centers (MRSEC) program [DMR 1120296]
- Energy Materials Center at Cornell (emc2), an Energy Frontier Research Center - U.S. Department of Energy, Office of Basic Energy Sciences [DESC0001086]
- American Chemical Society Division of Analytical Chemistry
- Eastman Chemical Co.
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 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 nonlinear 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.
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