2D P-doped carbon nitride as an effective artificial solid electrolyte interphase for the protection of Li anodes

Abstract

Metallic lithium plays an important role in the development of next-generation lithium metal-based batteries. However, the uncontrolled growth of lithium dendrites limits the use of lithium metal as an anode. In this context, a stable solid electrolyte interphase (SEI) is crucial for regulating dendrite formation, stability, and cyclability of lithium metal anodes. This article proposes an artificial protective layer of P-doped carbon nitride on the lithium anode surface to address these issues. A thin film of P-doped carbon nitride (CNP) was created through a simple drop-casting method using synthesized CNP powder, forming an artificial SEI on the lithium electrode. The resulting symmetric CNP-modified Li/Li cells exhibited remarkable cyclability with low overpotentials of around 40 mV over 500 cycles at a current density of 3 mA cm−2. Anode degradation and SEI composition were thoroughly studied for cycled electrodes to gain insight into the mechanisms underlying this modified surface. Furthermore, these CNP-modified anodes were successfully utilized in a Li–S coin cell battery, achieving high capacity and capacity retention at a high current density (1C). First-principles calculations indicate that P-doping in the carbon nitride structure significantly enhances the surface diffusion of lithium and promotes more homogeneous lithium plating.