Doped quasi-two-dimensional carbons with layer-stacked porous architecture and chemically functionalized surface are strongly appealing for high-energy supercapacitors, but there are daunting challenges to synthesize them through a cost-efficient and eco-friendly path. Herein, N/S dual-doped stacked carbon nanosheets (D-SCN) is first synthesized from coal tar pitch, a cheap coking by-product, beginning with a controlled molecular radical-polymerization initiated by 2,3-dimethyl-2,3-diphenylbutane, followed by a one-step carbonization-activation process in presence of potassium benzoate and N,N′-diphenylthiourea. As-obtained D-SCN with reasonable densification shares a well-designed layer-stacked topology texture, hierarchical interconnected porous structure and N/S dual-doped surface, which work together to harvest high supercapacitive performance. The D-SCN delivers a maximal specific capacitance of 458 F g^-1, which is considerably higher than most of previously reported for other carbon materials. As-assembled asymmetric all-solid-state supercapacitor with a wide voltage range of 0∼1.8 V takes on a volumetric energy density of 27 W h L^-1 at a power density of 296 W L^-1 with fading capacitance of merely 5.9% after 20000 cycles. The route advocated here for preparing pitch-based nanocarbons opens up new horizons in exploring large-scale preparation of electrode materials suitable for narrow spaces.

具有高能级超级电容器的具有层堆叠多孔结构和化学功能化表面的掺杂准二维碳极具吸引力，但通过成本有效且环保的途径合成它们却面临着艰巨的挑战。在此，首先从廉价的焦化副产物煤焦油沥青中合成N / S双掺杂叠层碳纳米片（D-SCN），首先由2,3-二甲基-2,3引发受控的分子自由基聚合-二苯基丁烷，然后在苯甲酸钾和N，N'-二苯基硫脲的存在下进行一步碳化活化过程。如此获得的具有合理致密化的D-SCN具有精心设计的层堆叠拓扑结构，分层互连的多孔结构和N / S双掺杂表面，它们共同发挥了很高的超级电容性能。^-1，这大大高于先前针对其他碳材料所报告的大多数。组装后的宽电压范围为0〜1.8 V的非对称全固态超级电容器在296 WL ^-1的功率密度下具有27 W h L ^-1的体积能量密度，经过衰减后的衰落电容仅为5.9％ 20000个周期。这里提倡的制备沥青基纳米碳的途径为探索大规模制备适用于狭窄空间的电极材料开辟了新的视野。