Demonstration of an Electrochemical Liquid Cell for Operando Transmission Electron Microscopy Observation of the Lithiation/Delithiation Behavior of Si Nanowire Battery Anodes

Journal Article · Wed Nov 13 04:00:00 EST 2013 · Nano Letters, 13(12):6106-6112

DOI:https://doi.org/10.1021/nl403402q· OSTI ID:1114094

Gu, Meng ^[1]; Parent, Lucas R. ^[2]; Mehdi, Beata L. ^[1]; Unocic, Raymond R. ^[3]; McDowell, Matthew T. ^[4]; Sacci, Robert L. ^[3]; Xu, Wu ^[1]; Connell, Justin G. ^[5]; Xu, Pinghong ^[2]; Abellan Baeza, Patricia ^[1]; Chen, Xilin ^[1]; Zhang, Yaohui ^[6]; Perea, Daniel E. ^[1]; Evans, James E. ^[1]; Lauhon, Lincoln ^[5]; Zhang, Jiguang ^[1]; Liu, Jun ^[1]; Browning, Nigel D. ^[1]; Cui, Yi ^[7]; Arslan, Ilke ^[1] ; Wang, Chong M. ^[1]

---

1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
2. Univ. of California, Davis, CA (United States)
3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
4. Stanford Univ., CA (United States)
5. Northwestern Univ., Evanston, IL (United States)
6. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Harbin Inst. of Technology (China)
7. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Over the last few years, in-situ transmission electron microscopy (TEM) studies of lithium ion batteries using an open-cell configuration have helped us to gain fundamental insights into the structural and chemical evolution of the electrode materials in real time. In the standard open-cell configuration, the electrolyte is either solid lithium oxide or an ionic liquid, which is point-contacted with the electrode. This cell design is inherently different from a real battery, where liquid electrolyte forms conformal contact with electrode materials. The knowledge learnt from open cells can deviate significantly from the real battery, calling for operando TEM technique with conformal liquid electrolyte contact. In this paper, we developed an operando TEM electrochemical liquid cell to meet this need, providing the configuration of a real battery and in a relevant liquid electrolyte. To demonstrate this novel technique, we studied the lithiation/delithiation behavior of single Si nanowires. Some of lithiation/delithation behaviors of Si obtained using the liquid-cell are consistent with the results from the open-cell studies. However, we also discovered new insights different from the open cell configuration - the dynamics of the electrolyte and, potentially, a future quantitative characterization of the SEI layer formation and structural and chemical evolution.

• Research Organization: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States), Environmental Molecular Sciences Laboratory (EMSL)
• Sponsoring Organization: USDOE
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 1114094
• Report Number(s): PNNL-SA--99250; 48164; 48106; KC0208010
• Journal Information: Nano Letters, 13(12):6106-6112, Journal Name: Nano Letters, 13(12):6106-6112 Journal Issue: 12 Vol. 13; ISSN 1530-6984
• Country of Publication: United States
• Language: English

Related Subjects

25 ENERGY STORAGE
Environmental Molecular Sciences Laboratory