Transforming coal tar pitch (CTP) into porous carbon nanosheets (PCNS) offers a dual advantage: maximizing the value of CTP while pioneering novel carbon materials. A key challenge in synthesizing pitch-based PCNS lies in the hydrophobic nature and polycondensation of polycyclic aromatic hydrocarbons (PAHs) in CTP, limiting the integration of water-soluble additives and the formation of desired pore structures. In this study, oxidation process, commonly used in preparing pitch-based carbon fibers, was introduced into the synthesis pitch-based PCNS to address the aforementioned challenges. Through oxidization modification, hydrophilic functional groups rich in O, N and P were introduced to PAHs, while macromolecules were partially broken down into smaller aromatic compounds. Following oxidation, the carbon nanosheet structure was successfully achieved through co-carbonization of oxidized CTP and urea, during which the structure-directing agent CN was generated in-situ. Moreover, the efficacy of oxidation modification in the formation of nanosheet structures was assessed by comparing the structures of porous carbon derived from CTP both pre- and post-oxidation. In final, pitch-based PCNS were used in supercapacitors. In three-electrode system, capacitance of PCNS attained 331.3 F/g at 0.5 A/g, and its response speed, capacitance retention rate and ion transfer speed were also excellent. For solid state supercapacitor, its energy density and cycle stability after 10,000 cycles were 8.3 Wh/kg and 92.4%, respectively.

中文翻译：

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通过氧化和原位模板策略收获沥青基碳纳米片用于全固态超级电容器

将煤焦油沥青 (CTP) 转化为多孔碳纳米片 (PCNS) 具有双重优势：最大化 CTP 的价值，同时开创新型碳材料。合成沥青基 PCNS 的一个关键挑战在于 CTP 中多环芳烃 (PAH) 的疏水性和缩聚作用，限制了水溶性添加剂的整合和所需孔结构的形成。在本研究中，将常用于制备沥青基碳纤维的氧化工艺引入到合成沥青基PCNS中以解决上述挑战。通过氧化改性，PAHs中引入了富含O、N、P的亲水性官能团，同时大分子被部分分解成更小的芳香族化合物。氧化后，通过氧化CTP和尿素的共碳化成功地获得了碳纳米片结构，在此过程中原位生成了结构导向剂CN。此外，通过比较氧化前和氧化后源自 CTP 的多孔碳的结构，评估了氧化改性在纳米片结构形成中的功效。最后，基于沥青的PCNS被用于超级电容器。在三电极体系中，PCNS在0.5 A/g下的电容达到331.3 F/g，并且其响应速度、电容保持率和离子转移速度也很优异。对于固态超级电容器，10,000次循环后的能量密度和循环稳定性分别为8.3 Wh/kg和92.4%。