Citation: Jing Zhang, Su Zhang, Qiqi Li, Linken Ji, Yutong Li, Yukang Ren, Xiaobei Zang, Ning Cao, Han Hu, Peng Liang, Zhuangjun Fan. Integrating high surface area and electric conductivity in activated carbon by in situ formation of the less-defective carbon network during selective chemical etching[J]. Acta Physico-Chimica Sinica, ;2025, 41(10): 100114. doi: 10.1016/j.actphy.2025.100114 shu

Integrating high surface area and electric conductivity in activated carbon by in situ formation of the less-defective carbon network during selective chemical etching

Jing Zhang ^{1, †} ,
Su Zhang ^{1, †,,} ,
Qiqi Li ¹ ,
Linken Ji ² ,
Yutong Li ³ ,
Yukang Ren ¹ ,
Xiaobei Zang ¹ ,
Ning Cao ¹ ,
Han Hu ^4,, ,
Peng Liang ^5,, ,
Zhuangjun Fan ¹

1.
Shandong Key Laboratory of Intelligent Energy Materials, School of Materials Science and Engineering, China University of Petroleum (East China), Qingdao 266580, Shandong Province, China
2.
Qingdao Huashijie Environment Technology Co., Ltd., Qingdao 266510, Shandong Province, China
3.
College of New Energy, China University of Petroleum (East China), Qingdao 266580, Shandong Province, China
4.
College of Chemistry and Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, Shandong Province, China
5.
College of Chemical and Biological Engineering, Shandong University of Science and Technology, Qingdao 266590, Shandong Province, China

Corresponding author: Su Zhang, suzhangs@163.com Han Hu, hhu@upc.edu.cn Peng Liang, liangpeng202@hotmail.com
Received Date: 10 April 2025
Revised Date: 2 June 2025
Accepted Date: 10 June 2025

Fund Project: the National Natural Science Foundation of China 52062046the National Natural Science Foundation of China 52302336the National Natural Science Foundation of China 22179145the Taishan Scholar Project of Shandong Province tsqn202306131the Taishan Scholar Project of Shandong Province tsqn202312123the Key Basic Research Projects of Natural Science Foundation of Shandong province ZR2019ZD51

Activated carbons are widely used as the electrode material for supercapacitors owing to its large surface area, good electric conductivity, and outstanding electrochemical stability. Improving the electric conductivity of activated carbon is crucial for promoting its electrochemical energy storage, but hard to achieve because well-developed pores usually break the continuous conductive network. To solve this problem, researchers have developed several methods, such as selection of highly-conjugated carbon precursors, high-temperature post-treatment, compositing with highly conductive nanocarbons, and local catalytic graphitization. However, these methods generally suffer from high cost, low efficiency, and sacrifice of specific surface area. Herein, we propose a selective chemical etching strategy to prepare activated carbon with both high surface area and electric conductivity using a mixture of pitch and polyacrylonitrile (PAN) as the precursor. Through systematic investigation of the activation behavior of pure pitch, pure PAN, and the composite precursors, we demonstrate that the PAN-derived carbon contains amorphous and crystallized components. During activation, the amorphous carbon is primarily etched away due to its high reactivity, leading to the in-situ formation of less-defective carbon as the entire conductive network. The optimized sample shows a surface area of 2773 m²·g⁻¹ and 2.6 times increased electric conductivity of 912 S·m⁻¹, outperforming most of the reported activated carbons. Furthermore, the strong cross-linking between pitch and PAN molecules through pre-oxidation leads to a higher activated carbon yield of 58% than the pure pitch-derived activated carbon (34%). The optimized cross-linking structure also allows the activator K⁺ to be adsorbed more easily in the carbon precursor, which enhances the activation efficiency. As a result, the embedded PAN simultaneously construct conductive network and promote activation efficiency, leading to the integration of high electric conductivity and surface area of the activated carbon. For aqueous supercapacitor application, at the high electrode mass loading of 10 mg·cm⁻², the optimized material shows remarkable areal capacitance (2.8 F·cm⁻² at 1 A·g⁻¹) and good rate performance (41% retention at 50 A·g⁻¹). The corresponding device shows high energy densities (10.9 Wh·kg⁻¹) and remarkable cycle stability (100% retention after 50000 cycles). The reason is that good electric conductivity enables high surface area utilization, significantly improved electric double-layer formation and ion transport kinetics. This work demonstrates the significant potential of highly conductive activated carbon for practical applications, and provides novel insights into the design of conductive activated carbon for advanced energy storage.
- Activated carbon,
- Electric conductivity,
- Surface area,
- Supercapacitor,
- Chemical etching
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沈阳化工大学材料科学与工程学院沈阳 110142