Rights statement: This is the peer reviewed version of the following article: B. K. Antonopoulos, F. Maglia, F. Schmidt-Stein, J. P. Schmidt, H. E. Hoster, Batteries & Supercaps 2018, 1, 110 which has been published in final form at http://onlinelibrary.wiley.com/doi/10.1002/batt.201800029/abstract This article may be used for non-commercial purposes in accordance With Wiley Terms and Conditions for self-archiving.
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Research output: Contribution to Journal/Magazine › Journal article › peer-review
Formation of the Solid Electrolyte Interphase at Constant Potentials : a Model Study on Highly Oriented Pyrolytic Graphite. / Antonopoulos, Byron Konstantinos; Maglia, Filippo; Schmidt-Stein, Felix et al.
In: Batteries & Supercaps, Vol. 1, No. 3, 09.2018, p. 110-121.Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - Formation of the Solid Electrolyte Interphase at Constant Potentials
T2 - a Model Study on Highly Oriented Pyrolytic Graphite
AU - Antonopoulos, Byron Konstantinos
AU - Maglia, Filippo
AU - Schmidt-Stein, Felix
AU - Hoster, Harry Ernst
AU - Schmidt, Jan Philipp
N1 - This is the peer reviewed version of the following article: B. K. Antonopoulos, F. Maglia, F. Schmidt-Stein, J. P. Schmidt, H. E. Hoster, Batteries & Supercaps 2018, 1, 110 which has been published in final form at http://onlinelibrary.wiley.com/doi/10.1002/batt.201800029/abstract This article may be used for non-commercial purposes in accordance With Wiley Terms and Conditions for self-archiving.
PY - 2018/9
Y1 - 2018/9
N2 - The solid electrolyte interphase (SEI) on graphite anodes is a key enabler for rechargeable lithium ion batteries (LIBs). It ensures that only Li+ ions and no damaging electrolyte components enter the anode and hinders electrolyte decomposition. Its growth should be confined to the initial SEI formation process and stop once the battery is in operation to avoid capacity/power loss. In technical LIB cells, the SEI is formed at constant current, with the potential of the graphite anode slowly drifting from higher to lower voltages. SEI formation rate, composition, and structure depend on the potential and on the chemical properties of the anode surface. Here, we characterize SEIs formed at constant potentials on the chemically inactive basal plane of highly oriented pyrolytic graphite (HOPG). X‐ray photoemission spectroscopy (XPS) detects carbonate‐species only at lower formation potentials. Cyclic voltammetry (CV) and Electrochemical Impedance Spectroscopy (EIS) with Fc/Fc+ as an electrochemical probe demonstrate how the formation potential influences ion transport and electrochemical kinetics to and at the anode surface, respectively. Breaking the EIS data down to a Distribution of Relaxation Times (DRT) reveals distinct kinetics and transport related peaks with varying Arrhenius‐type temperature dependencies. We discuss our findings in the context of previous electrochemical studies and existing SEI models and of SEI formation protocols suitable for industry.
AB - The solid electrolyte interphase (SEI) on graphite anodes is a key enabler for rechargeable lithium ion batteries (LIBs). It ensures that only Li+ ions and no damaging electrolyte components enter the anode and hinders electrolyte decomposition. Its growth should be confined to the initial SEI formation process and stop once the battery is in operation to avoid capacity/power loss. In technical LIB cells, the SEI is formed at constant current, with the potential of the graphite anode slowly drifting from higher to lower voltages. SEI formation rate, composition, and structure depend on the potential and on the chemical properties of the anode surface. Here, we characterize SEIs formed at constant potentials on the chemically inactive basal plane of highly oriented pyrolytic graphite (HOPG). X‐ray photoemission spectroscopy (XPS) detects carbonate‐species only at lower formation potentials. Cyclic voltammetry (CV) and Electrochemical Impedance Spectroscopy (EIS) with Fc/Fc+ as an electrochemical probe demonstrate how the formation potential influences ion transport and electrochemical kinetics to and at the anode surface, respectively. Breaking the EIS data down to a Distribution of Relaxation Times (DRT) reveals distinct kinetics and transport related peaks with varying Arrhenius‐type temperature dependencies. We discuss our findings in the context of previous electrochemical studies and existing SEI models and of SEI formation protocols suitable for industry.
KW - SEI Formation
KW - Highly Oriented Pyrolitic Graphite
KW - Model Electrode Surface
KW - electrochemistry
KW - materials science
KW - outer sphere reaction
U2 - 10.1002/batt.201800029
DO - 10.1002/batt.201800029
M3 - Journal article
VL - 1
SP - 110
EP - 121
JO - Batteries & Supercaps
JF - Batteries & Supercaps
SN - 2566-6223
IS - 3
ER -