Effects of external pressure on cycling performance of silicon-based lithium-ion battery: modelling and experimental validation.

Controlling the stress state of electrodes during electrochemical cycling can have a positive effect on the cycling performance of lithium-ion battery. In this work, we study the cycling performance of silicon-based lithium-ion half cells under the action of pressure in a range of 0.1 to 0.4 MPa. The cycling performance of the silicon-based lithium-ion half cells increases first with increasing the pressure to 0.2 MPa and then decreases with further increasing the pressure. The analysis of the surface morphologies of cycled electrodes reveals that applying a pressure of 0.2 MPa leads to the formation of fine electrode surface with the least surface cracks after the silicon-based lithium-ion half cells are cycled for 50 times, which supports the dependence of the cycling performance of the lithium-ion half cells on the pressure. The numerical results from the single particle model reveal that applying pressure can tune the stress state in a single electrode particle and reduce the tensile stress. However, the numerical results from the two-particle model point to that applying pressure can introduce tensile stress in the electrode particles due to contact deformation. Suitable pressure applied onto a lithium-ion battery is needed in order to improve the cycling performance of the lithium-ion battery without causing detrimental effects.