
Silicon presents itself as a high-capacity anode material for lithium-ion batteries with a promising future. The high ability for lithiation comes along with massive volume changes and a problematic voltage hysteresis, causing reduced efficiency, detrimental heat generation, and a complicated state-of-charge estimation. During slow cycling, amorphous silicon nanoparticles show a larger voltage hysteresis than after relaxation periods. Interestingly, the voltage relaxes for at least several days, which has not been physically explained so far. We apply a chemo-mechanical continuum model in a core-shell geometry interpreted as a silicon particle covered by the solid-electrolyte interphase to account for the hysteresis phenomena. The silicon core (de)lithiates during every cycle while the covering shell is chemically inactive. The visco-elastoplastic behavior of the shell explains the voltage hysteresis during cycling and after relaxation. We identify a logarithmic voltage relaxation, which fits with the established Garofalo law for viscosity. Our chemo-mechanical model describes the observed voltage hysteresis phenomena and outperforms the empirical Plett model. In addition to our full model, we present a reduced model to allow for easy voltage profile estimations. The presented results support the mechanical explanation of the silicon voltage hysteresis with a core-shell model and encourage further efforts into the investigation of the silicon anode mechanics.
Chemical Physics (physics.chem-ph), Condensed Matter - Materials Science, Silicon Voltage Relaxation, Materials Science (cond-mat.mtrl-sci), FOS: Physical sciences, Solid-Electrolyte Interphase (SEI), SEI Mechanics, Physics - Applied Physics, Applied Physics (physics.app-ph), Voltage Relaxation, Lithium-Ion Batteries, Voltage Hysteresis, Chemo-Mechanical Core-Shell Model, Silicon Anode, Visco-elastoplastic Model, Physics - Chemical Physics, Garofalo Viscosity, Silicon-SEI Mechanics
Chemical Physics (physics.chem-ph), Condensed Matter - Materials Science, Silicon Voltage Relaxation, Materials Science (cond-mat.mtrl-sci), FOS: Physical sciences, Solid-Electrolyte Interphase (SEI), SEI Mechanics, Physics - Applied Physics, Applied Physics (physics.app-ph), Voltage Relaxation, Lithium-Ion Batteries, Voltage Hysteresis, Chemo-Mechanical Core-Shell Model, Silicon Anode, Visco-elastoplastic Model, Physics - Chemical Physics, Garofalo Viscosity, Silicon-SEI Mechanics
| selected citations These citations are derived from selected sources. This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically). | 4 | |
| popularity This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network. | Top 10% | |
| influence This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically). | Average | |
| impulse This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network. | Average |
