Developing highly efficient, sustainable carbon cathodes is essential for emerging Zn-ion hybrid supercapacitors (ZICs). Herein, lignin's novel chemical modification (amination) has been developed to produce high quantity pyrrolic-N moieties as active sites. Furthermore, chemically modified amine moieties in lignin are vital as a natural self-activating template to generate hierarchical porosity in the 2D (graphene-like) architecture with exceedingly high surface area (2926.4 m²g⁻¹). The rationally introduced dominated pyrrolic-N moieties boost the Zn-ion storage capacity and reaction kinetics due to the dual energy storage mechanism and efficient charge transfer between pyrrolic-N and Zn⁺² ions. Furthermore, the pyrrolic-N species are energetically favorable for the adsorption of Zn⁺² ions by the formation of N-Zn⁺² chemical bonds. Besides, the nitrogen oxides reduce the intrinsic resistance and induce a more polarized surface, resulting in high wettability and efficient transfer of electrolytes into the pores of hydrophobic carbon materials. Subsequently, the chemically modified lignin-derived activated carbon material (Chem-ACM) as a cathode in ZICs delivers a high capacity of 161.2 mA h g⁻¹ at 1 A g⁻¹ with the admirable energy density of 106.7 W h kg⁻¹ at 897 W kg⁻¹ and excellent retention capacity (94%) after 10,000 cycles. Mainly, the assembled quasi solid-state ZICs using Chem-ACM retains the remarkable storage capacity (202 mA h g⁻¹ at 0.2 Ag⁻¹) even at a high bending angle. Notably, the Chem-ACM has been further employed in symmetric supercapacitors as an electrode, and it displays exceptional specific capacitance of 354 Fg⁻¹ at 0.5 Ag⁻¹ with tremendous energy (43.5 W h kg⁻¹) and the power density (0.53 kW kg⁻¹). Additionally, the charge storage capability of Chem-ACM is positively dependent on high nitrogen contents, and it is extrapolated that pyrrolic-N moieties are dominant active sites. Hence, the designed amination-assisted biocarbon synthesis provides a new way to prepare high nitrogen-containing biocarbon for ZICs and further understand pyrrolic-N species' impact on Zn-ion storage.

开发高效、可持续的碳阴极对于新兴的锌离子混合超级电容器 (ZIC) 至关重要。在此，木质素的新型化学修饰（胺化）已被开发出来以产生大量的吡咯-N 部分作为活性位点。此外，木质素中经过化学修饰的胺部分作为天然自激活模板至关重要，可在具有极高表面积 (2926.4 m 2 g -1 ) 的 2D（类石墨烯）结构中生成^分级孔隙^率。由于吡咯-N 和 Zn ^{+2之间的双重储能机制和有效电荷转移，合理引入的主导吡咯-N 部分提高了 Zn 离子存储容量和反应动力学}离子。此外，吡咯-N 物种通过形成N -Zn ⁺²化学键在能量上有利于 Zn ^{+2离子的吸附。}此外，氮氧化物降低了本征电阻并诱导了更极化的表面，从而导致高润湿性和电解质有效转移到疏水碳材料的孔隙中。^{随后，化学改性的木质素衍生活性炭材料(} Chem-ACM) 作为 ZIC 的阴极，在 1 A g ^-1时提供 161.2 mA h g -1 的高^容量，在897 瓦公斤^-110,000 次循环后具有出色的保留容量 (94%)。主要是，使用 Chem-ACM 组装的准固态 ZIC即使在高弯曲角度下也能保持显着的存储容量（在 0.2 Ag ^{-1时为 202 mA h g -1 ）。}值得注意的是，Chem-ACM 已进一步用于对称超级电容器作为电极，它在 0.5 Ag ^{-1时显示出 354 Fg -1}的特殊电容，具有巨大的能量（43.5 W h kg ^-1）和功率密度（0.53千瓦公斤^-1). 此外，Chem-ACM 的电荷存储能力与高氮含量正相关，据推测吡咯-N 部分是主要的活性位点。因此，设计的胺化辅助生物碳合成为 ZICs 制备高含氮生物碳提供了一种新方法，并进一步了解吡咯-N 物种对锌离子储存的影响。