Precisely Engineered Nitrogen-Doped Hierarchical Porous Carbon from Lignin for High-Rate and Ultra-Stable Supercapacitors
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The development of high-performance and sustainable carbon electrodes is increasingly important for next-generation supercapacitors, yet controlling heteroatom doping and hierarchical pore evolution in biomass-derived carbons remains a key challenge. Lignin, as an abundant aromatic biopolymer, offers a structurally rich platform for designing functional carbons, but its rigid cross-linked architecture limits precise pore regulation and efficient nitrogen incorporation. In this work, nitrogen-doped hierarchical porous carbons were engineered from enzymatically treated lignin through a synergistic urea-assisted nitrogen doping and KOH activation strategy. The urea–KOH co-activation drives the coordinated evolution of micropores and mesopores. This approach yields an optimized carbon material possessing a high BET surface area of 2569 m2 g−1, an interconnected micro–mesoporous architecture, and a favorable distribution of pyridinic, pyrrolic, and graphitic nitrogen species. The engineered pore hierarchy is correlated with enhanced ion transport kinetics, as evidenced by a high b value of 0.99 and a capacitive contribution of 98.5% at 100 mV s−1; nitrogen functionalities introduce redox-active sites and improve interfacial wettability. As a result, the selected material delivers a high specific capacitance of 221 F g−1 at 0.5 A g−1, strong rate capability with 84.4% retention at 20 A g−1, and excellent cycling durability with 90.7% capacitance retention after 50,000 cycles. This study demonstrates a potentially mechanistically informed, scalable pathway for coupling enzymatic structural regulation with chemical activation, offering a sustainable route for transforming lignin into high-value carbon electrodes suitable for advanced supercapacitor applications.