Intercalated ion tuning of the cross-plane thermal transport properties of graphite

The effects of the intercalated ion concentration on the cross-plane thermal conductivity and the thermal boundary conductance in the graphite/lithiated graphite interface are investigated from molecular dynamics simulations. At low ion concentration, the cross-plane thermal conductivity of the lithiated graphite is lower than that of the pristine graphite. However, as the intercalated ion concentration increases, the cross-plane thermal conductivity increases rapidly, even exceeding that of the pristine graphite at high ion concentration. By analyzing the variations of the cross-plane elastic constants and phonon dispersion relation with the intercalated ion concentration, it is found that the intercalated ions significantly increase the phonon irradiation heat flux along the cross-plane direction. Our study further shows that the variation of the intercalated ion concentrations can also modulate the thermal boundary conductance in the graphite/lithiated graphite interface. The non-equilibrium molecular dynamics simulations show that the thermal boundary conductance between graphite and lithiated graphite decreases as the lithiation level increases, which would worsen the thermal performance of Li-ion batteries. A one-dimensional atomic chain model is proposed to elaborate on how the effective spring stiffness of material influences the interfacial transmission of phonons with different frequencies. This work provides a quantitative calculation of the cross-plane thermal conductivity and thermal boundary conductance in intercalated graphite samples and is also extremely important for the thermal management and structural design of lithium-ion batteries.