In Situ Measurement of Solid Electrolyte Interphase Evolution on Silicon Anodes Using Atomic Force Microscopy

Journal Article · Mon Apr 18 04:00:00 EDT 2016 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201600099· OSTI ID:1338190

Yoon, Insun ^[1]; Abraham, Daniel P. ^[2]; Lucht, Brett L. ^[3]; Bower, Allan F. ^[1]; Guduru, Pradeep R. ^[1]

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1. School of Engineering, Brown University, Providence RI 02912 USA
2. Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne IL 60439 USA
3. Department of Chemistry, University of Rhode Island, Kingston RI 02881 USA

In situ measurements of the growth of solid electrolyte interphase (SEI) layer on silicon and the lithiation-induced volume changes in silicon in lithium ion half-cells are reported. Thin film amorphous silicon electrodes are fabricated in a configuration that allows unambiguous separation of the total thickness change into contribution from SEI thickness and silicon volume change. Electrodes are assembled into a custom-designed electrochemical cell, which is integrated with an atomic force microscope. The electrodes are subjected to constant potential lithiation/delithiation at a sequence of potential values and the thickness measurements are made at each potential after equilibrium is reached. Experiments are carried out with two electrolytes—1.2 m lithium hexafluoro-phosphate (LiPF6) in ethylene carbonate (EC) and 1.2 m LiPF6 in propylene carbonate (PC)—to investigate the influence of electrolyte composition on SEI evolution. It is observed that SEI formation occurs predominantly during the first lithiation and the maximum SEI thickness is ≈17 and 10 nm respectively for EC and PC electrolytes. This study also presents the measured Si expansion ratio versus equilibrium potential and charge capacity versus equilibrium potential; both relationships display hysteresis, which is explained in terms of the stress–potential coupling in silicon.

• Research Organization: Argonne National Lab. (ANL), Argonne, IL (United States)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
• DOE Contract Number: AC02-06CH11357
• OSTI ID: 1338190
• Journal Information: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 12 Vol. 6; ISSN 1614-6832
• Publisher: Wiley
• Country of Publication: United States
• Language: English

Related Subjects

36 MATERIALS SCIENCE