Tuning Li + and Na + Functionality in Renewable Carbon Electroactive Material Through Site‐Specific Nanostructural Disorder

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Abstract
Understanding the hybrid structural characteristics of carbon remains a significant challenge, hindering the development of clear design principles for optimizing electrode materials in energy storage systems—particularly in lithium‐ion (Li‐ion) and sodium‐ion (Na‐ion) batteries. Traditionally, the localized structural disorder and intrinsic porosity of carbon have been regarded as the primary contributors to its high storage capacity in Na‐ion batteries. However, our investigation reveals that the hybrid structural features of carbon play a more dominant role in enhancing energy storage performance in Li‐ion systems compared to Na‐ion counterparts. Through comprehensive materials characterization and electrochemical analysis, we establish a direct correlation between the local microstructural attributes of carbon and its ion storage kinetics which elucidate the distinct ion‐storage mechanisms that differentiate Li‐ion from Na‐ion systems. This study reinforces our findings that configurational defects are crucial for achieving high initial storage capacity in carbon crafted with mixed‐phase structures, but the in‐plane size of nano‐layered microdomains plays a key role in ensuring long‐term stable storage capacity in rechargeable batteries.

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