In Situ Alkali Metal Exfoliation‐Coupled Dilute CO ₂ Electrolysis to Synthesize Interlayer‐Expanded Graphite for High‐Rate Lithium Storage

ABSTRACT Converting CO 2 into ideal carbon anode materials for fast lithium storage brings a win‐win prospect toward energy and environment domains. Here, we propose a one‐pot stepwise strategy to synthesize expanded d ‐spacing (up to 0.405 nm) graphite by direct electroreduction of dilute CO 2 (e.g., 10 vol%, close to practical industrial flue gas) in molten electrolytes, where the as‐formed CO 2 ‐derived graphite with pristine interlayer spacing was enlarged by the sequential in situ exfoliation of alkali metals. Owing to the predominant thermodynamic tendency, dilute CO 2 was preferentially electro‐transformed into carbon materials at a promising current density of 100 mA/cm 2 . Serving as a LIBs anode, the obtained graphite with expanded d ‐spacing exhibited a relatively high lithium storage capacity (152 mAh/g) at a high charge/discharge current density of 2000 mA/g, fivefold compared with that of commercial graphite, reaching a retention rate of 91% after 500 cycles. This work provides insights on rational design of high‐rate lithium storage anode for next‐generation LIBs industry with a lower carbon footprint.