The CK bond plays a significant role in stabilizing the Na‐K (NaK) alloy electrodes due to the enhancive interfacial affinity. In this study, a method for constructing semi‐solid K metal electrodes with rich CK bonds by in situ replacement of N‐doped carbon nanotubes (CNT) and liquid NaK alloy is proposed. Based on the in situ infrared thermal imaging technique combined with heat calculation, X‐ray photoelectron spectroscopy elemental analysis, and reaction thermodynamic calculation, graphite‐N, which is widely distributed on the wall of CNT, offers plenty of replacement sites for forming CK bonds. Due to the rich bonds, the amount of CNT sharply reduces in dendrite‐free semi‐solid CNT@NaK electrodes and the activity of NaK alloy raises to ≈90%. This discovery provides a new idea for establishing dendrite‐free anodes for K metal batteries.
Primary electrodeposition is an accepted strategy to elucidate the nucleation and growth kinetics of metal electrodes. Nevertheless, when confronted with the phase transition process caused by bi-active metals such as NaK liquid alloys, the research process becomes complex and elusive. Herein, we have reduced the intricate issues to relatively simple initial alloying behaviors. Two exchange diffusion mechanisms of the Na atom embedded in K crystals and K atom embedded in Na crystals are investigated by first-principles density functional theory (DFT) calculation and mechanical simulation. As a result, the process of embedding the Na atom in K crystals shows a better thermodynamic stability and lower activation barrier and structural stress than those of the other. The abovementioned conclusions are further proved by stepwise Na and K electrodeposition experiments, and the prepared NaK alloy electrode displays excellent electrochemical performance. Our findings correlate the original alloying mechanism model specification with electrodeposition experimental verification and provide strategies to achieve controllable NaK electrode construction.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.