Using a cyclocarbon additive as a cyclone separator to achieve fast lithiation and delithiation without dendrite growth in lithium-ion batteries

Abstract

Carbon materials are widely used for reversible lithium uptake in the anode of lithium-ion batteries. Nevertheless, the challenge of uncontrollable dendrite deposition during fast charge–discharge cycles remains a grand hurdle. Various strategies have been explored to prevent detrimental heterogeneous dendrite metal deposits, such as interface engineering and electrolyte modification, but they often compromise the reverse diffusion freedom of Li⁺ ions during discharging and are incompatible with the most mainstream use of graphite as an anode material. Here, we propose the incorporation of a novel carbon allotrope of cyclocarbon as a potential additive in the anode. In contrast to conventional carbon materials, density functional theory calculations reveal that cyclocarbon has a much higher affinity for Li atoms than Li⁺ ions, even surpassing the inherent cohesion of Li atoms, due to the charge transfer from the 2s orbital of Li atoms to the unique in-plane π orbital of cyclocarbon. Furthermore, ab initio molecular dynamics simulations show that Li⁺ ions can shuttle freely back and forth across cyclocarbon, whereas the lithiation process for Li atoms occurs rapidly within picoseconds. The delithiation of Li atoms within cyclocarbon follows a voltage-gated mechanism that is effectively controlled by an external electric field of 3 V nm⁻¹. Remarkably, cyclocarbon exhibits potential compatibility with commercialized graphite electrodes via the π–π interaction and also can be extended to sodium-ion and potassium-ion batteries. These distinct compatibility, scalability and electrochemical properties of cyclocarbon provide a new avenue to realize both safety and ultrafast rechargeable performance of ion batteries.