Enhanced Interfacial Kinetics of Carbon Monolith Boosting Ultrafast Na-Storage.

Slow ion kinetics of negative electrode materials is the main factor of limiting fast charge and discharge of batteries. Sluggish Na+ kinetics property leads to large electrode polarization, resulting in poor rate and cyclic performances. Herein, an electrode of ultrasmall tin nanoparticles decorated in N, S codoped carbon monolith (TCM) with exceptional high-rate capability and ultrastable cycling behavior for Na-storage is reported. The resulted TCM electrode exhibits an extremely high retention of 96% initial charge capacity after 500 cycles at a current density of 500 mA g-1 . Significantly, when the current density is elevated to an ultrahigh rate of 5000 mA g-1 , a high reversible capacity of 228 mAh g-1 after the 2000th cycle is still maintained. More importantly, the stable and fast Na-storage of TCM is investigated and understood by experimental characterizations and kinetics calculations, including interfacial ion/electron transport behavior, ion diffusion, and quantitative pseudocapacitive analysis. These investigations elucidate that the TCM shows improved ion/electron conductivity and enhanced interfacial kinetics. An entirely new perspective to deep insights into the fast ion/electron transport mechanisms revealed by interfacial kinetics of sodiation/desodiation, which contributes to the profound understanding for developing fast charging/discharging and long-term stable electrodes in sodium-ion batteries, is provided.