Constructing high-loading (>10 mg/cm²) carbon-based electrode materials is an effective way to simultaneously boost the gravimetric/volumetric energy density and power density of capacitors. However, porous carbon materials usually have high defect structures, low compaction density, and low graphitization degree, which severely hinder their electron/ion transport rates at high mass loading, thereby deteriorating the electrochemical performance. Thus, we first propose to construct short-range ordered porous carbon materials with high compaction density to enhance the detailed electrochemical performance without affecting the electron/ion transport rates. Herein, S, N codoped porous carbon (3SN-NAC-800) with a large specific surface area, high compaction density, and abundant short-range ordered structures was prepared by the confined-region activation method, in which needle coke was used as precursor, thiourea as the dopant, and KOH as the activator under 10 MPa pressure. The 3SN-NAC-800 electrode with 4 mg/cm² exhibits high capacities of 267.2 and 229.7 F/g under 2 and 50 A/g, respectively, and 92.9% capacitance retention for 20,000 cycles. When the mass loading was increased to 8, 12, and 14 mg/cm², it still exhibited high capacities of 260.4, 257.5, and 250.4 F/g at 2 A/g, respectively. Besides, the electrode with 12 mg/cm² shows high gravimetric and areal capacitance values of 197.3 F/g and 2367.12 mF/cm² at 40 A/g, respectively, as well as 90.98% capacity retention for 20,000 cycles, showing excellent rate capability and cycling stability. Furthermore, it exhibits a maximum energy density of 0.11 mWh/cm² at 2.97 mW/cm², and a maximum power density of 87.6 mW/cm² at 0.044 mWh/cm². This work demonstrates an efficient strategy to prepare short-range ordered porous carbon materials for high-mass-loading capacitors.

中文翻译：

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由限域激活策略衍生的短程有序多孔碳在超级电容器中表现出优异的高负载性能

构建高负载量（>10 mg/cm ²）碳基电极材料是同时提高电容器重量/体积能量密度和功率密度的有效方法。然而，多孔碳材料通常具有高缺陷结构、低压实密度和低石墨化度，这严重阻碍了其在高质量负载下的电子/离子传输速率，从而恶化了电化学性能。因此，我们首先提出构建具有高压实密度的短程有序多孔碳材料，以在不影响电子/离子传输速率的情况下增强详细的电化学性能。本文以针状焦为原料，采用限域活化法制备了具有大比表面积、高压实密度和丰富的短程有序结构的S、N共掺杂多孔碳（3SN-NAC-800）。以硫脲为前驱体、硫脲为掺杂剂、KOH为活化剂，在10 MPa压力下制备。 4 mg/cm ²的3SN-NAC-800电极在2和50 A/g下分别表现出267.2和229.7 F/g的高容量，以及20,000次循环后92.9%的电容保持率。当质量负载增加至8、12和14 mg/cm ²时，其在2 A/g下仍分别表现出260.4、257.5和250.4 F/g的高容量。此外，12 mg/cm ²的电极在40 A/g下表现出较高的重量电容值和面积电容值，分别为197.3 F/g和2367.12 mF/cm ²，以及20,000次循环后的容量保持率为90.98%，表现出优异的倍率能力和循环稳定性。此外，其在2.97mW/cm ²处表现出0.11mWh/cm ²的最大能量密度，在0.044mWh/cm ^{2处表现出87.6mW/cm 2}的最大功率密度。这项工作展示了一种制备用于高质量负载电容器的短程有序多孔碳材料的有效策略。