TY - JOUR

T1 - Solid Electrolyte Interphase

T2 - Can faster formation at lower potentials yield better performance?

AU - Antonopoulos, Byron Konstantinos

AU - Stock, Christoph

AU - Maglia, Filippo

AU - Hoster, Harry Ernst

N1 - This is the author’s version of a work that was accepted for publication in Electrochimica Acta. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Electrochimica Acta, 269, 2018 DOI: 10.1016/j.electacta.2018.03.007

PY - 2018/4/10

Y1 - 2018/4/10

N2 - To make a Lithium Ion Battery (LIB) reliably rechargeable over many cycles, its graphite-based negative electrode requires the solid electrolyte interphase (SEI) as a protection layer. The SEI is formed through chemical and particularly electrochemical side reactions of electrolyte components in the first charging cycle(s) after manufacturing of a LIB. The SEI ideally serves two purposes: (i) act as a sieve permeable to Li ions but not to other electrolyte components and (ii) passivate the electrode against further electrolyte decomposition. Core element of conventional SEI formation is a lengthy, low-current galvanostatic charging step, which due to its time consumption contributes heavily to cell manufacturing costs. Here, we report on some non-conventional SEI formation protocols for composite carbon electrodes, inspired by recent experimental findings at smooth model electrodes. Acknowledging that the SEI forms in two main steps, taking place in a high-potential and a low-potential region, respectively, we demonstrate that less time spent in the high-potential region not only makes the process faster but even yields SEIs with superior kinetic properties. We tentatively explain this via basic rules of thin film growth and the role of grain boundaries for ion transport. We also report on the positive influence of multi-frequency potential modulations applied between high-potential and low-potential formation. Given that any new cell chemistry in principle requires its own tailor-made formation process, technologic success of future LIB cells will benefit from a systematic, well-understood toolbox of formation protocols. This paper is meant as a first step, highlighting potentially low-hanging fruits, but also flagging the demand for further systematic studies on model systems and on commercially manufactured cells.

AB - To make a Lithium Ion Battery (LIB) reliably rechargeable over many cycles, its graphite-based negative electrode requires the solid electrolyte interphase (SEI) as a protection layer. The SEI is formed through chemical and particularly electrochemical side reactions of electrolyte components in the first charging cycle(s) after manufacturing of a LIB. The SEI ideally serves two purposes: (i) act as a sieve permeable to Li ions but not to other electrolyte components and (ii) passivate the electrode against further electrolyte decomposition. Core element of conventional SEI formation is a lengthy, low-current galvanostatic charging step, which due to its time consumption contributes heavily to cell manufacturing costs. Here, we report on some non-conventional SEI formation protocols for composite carbon electrodes, inspired by recent experimental findings at smooth model electrodes. Acknowledging that the SEI forms in two main steps, taking place in a high-potential and a low-potential region, respectively, we demonstrate that less time spent in the high-potential region not only makes the process faster but even yields SEIs with superior kinetic properties. We tentatively explain this via basic rules of thin film growth and the role of grain boundaries for ion transport. We also report on the positive influence of multi-frequency potential modulations applied between high-potential and low-potential formation. Given that any new cell chemistry in principle requires its own tailor-made formation process, technologic success of future LIB cells will benefit from a systematic, well-understood toolbox of formation protocols. This paper is meant as a first step, highlighting potentially low-hanging fruits, but also flagging the demand for further systematic studies on model systems and on commercially manufactured cells.

KW - SEI formation

KW - Li-ion battery

KW - pre-charge

KW - composite carbon electrodes

KW - Cyclic Voltammetry

U2 - 10.1016/j.electacta.2018.03.007

DO - 10.1016/j.electacta.2018.03.007

M3 - Journal article

VL - 269

SP - 331

EP - 339

JO - Electrochimica Acta

JF - Electrochimica Acta

SN - 0013-4686

ER -