Electron transport properties of heterogeneous interfaces in solid electrolyte interphase on lithium metal anodes (2501.12686v1)

Abstract: In rechargeable batteries, electron transport properties of inorganics in the solid-electrolyte interphase (SEI) critically determine the safety, lifespan and capacity loss of batteries. However, the electron transport properties of heterogeneous interfaces among different solid inorganics in SEI have not been studied experimentally or theoretically yet, although such heterogeneous interfaces exist inevitably. Here, by employing non-equilibrium Green's function (NEGF) method, we theoretically evaluated the atomic-scale electron transport properties under bias voltage for LiF/Li2O interfaces and single-component layers of them, since LiF and Li2O are common stable inorganics in the SEI. We reveal that heterogeneous interfaces orthogonal to the external electric-field direction greatly impede electron transport in SEI, whereas heterogeneous parallel-orientated interfaces enhance it. Structural disorders induced by densely distributed interfaces can severely interfere with electron transport. For each component, single-crystal LiF is highly effective to block electron transport, with a critical thickness of 2.9 nm, much smaller than that of Li2O (19.0 nm). This study sheds a new light into direct and quantitative understanding of the electron transport properties of heterogeneous interfaces in SEI, which holds promise for the advancement of a new generation of high-performance batteries.