Cobalt-Catalyzed Carbonization Incorporating Disordered Defects in Ordered Graphitic Domains for Fast and Ultrastable...

Carbonaceous materials featuring both ordered graphitic structure and disordered defects hold great promise for high-performance K-ion batteries (KIBs) due to the concurrent advantages of high electronic conductivity, fast and reversible K⁺ intercalation/deintercalation, and abundant active K⁺ storage sites. However, it has been a lingering problem and remains a big challenge because graphitization and defects are intrinsic trade-off properties of carbonaceous materials. Herein, for the first time, we propose a cobalt-catalyzed carbonization strategy to fabricate porous carbon nanofibers that incorporate disordered defects in graphitic domain layers (PCNFs-DG) for fast and durable K⁺ storage. The Co catalyst not only ensures the formation of highly graphitized carbon shells around the Co particles but also introduces nanopores and doping defects in the following catalyst removal process. This idea of architecting defected-ordered graphitic carbon engineering guarantees fast reaction kinetics as well as structural stability with negligible interlayer expansion/contraction owing to the uncompromised electronic conductivity, expanded interlayer spacing, and regulated K⁺ storage mechanism. These appealing features translate to a high reversible capacity of 318.5 mAh g^-1 at 100 mA g^-1 and ultrahigh stability with almost 100% capacity retention over 2000 cycles in KIBs. This work puts in perspective that defected and ordered carbonaceous materials could be simultaneously achieved, advancing their performance for next-generation energy storage systems.