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Effect of graphitic structure on electrochemical ion intercalation into positive and negative electrodes

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Abstract

Commercially activated carbons are known for their high specific surface areas and low pack densities, thus giving a poor volumetric capacitance for supercapacitors. Here, nonporous pyrolyzed graphite oxides with high pack densities and controllable graphitic structures were prepared through a facile oxidation-heat treatment. XRD, Raman, SEM, and TEM were used to characterize the textural properties and morphologies of these materials. Galvanostatic charge–discharge and cyclic voltammetry revealed that the voltage-driven electrochemical ion intercalation process is, in fact, highly dependent on the graphitic structure. Less graphitized materials with larger interlayer spacings are more easily electrochemically activated, while a more rigid graphitic structure proves to be more difficult. After adequate electrochemical activation, abundant ion-accessible sites were created for charge storage, and the cell-specific capacitance dramatically increased from 3.5 to 23 F/g. The intercalation behaviors of TEA+ and BF4 − were separately studied. The results revealed that, due to its smaller anion size, BF4 − displayed superior intercalation capability as well as higher specific capacitance on the positively polarized electrode after electrochemical activation. Therefore, through optimizing the graphitic structure and the EA conditions, a high volumetric capacitance can be achieved.

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Acknowledgments

This work was partly supported by MOST (2014CB239702), National Science Foundation of China (no. 51302083, no. 51172071, no. 51272077), Fundamental Research Funds for the Central Universities, Shanghai Pujiang Program, and Program of Shanghai Subject Chief Scientist (B type, no 13XD1424900). Chuanfang Zhang acknowledges the financial support of Chinese Scholarship Council. Zheng Ling is thanked for useful discussions. Prof. Yury Gogotsi (Drexel University) is acknowledged for manuscript revision and helpful discussions.

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Authors and Affiliations

  1. State Key Laboratory of Chemical Engineering, Department of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China

    Chuanfang Zhang, Jitong Wang, Donghui Long, Licheng Ling & Wenming Qiao

  2. A.J. Drexel Nanomaterials Institute, Department of Materials Science and Engineering, Drexel University, Philadelphia, PA, 19104, USA

    Chuanfang Zhang & Amanda Pentecost

  3. Titan Chem Co., LTD, Shanghai, 200237, China

    Yingbo Xie

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  1. Chuanfang Zhang
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  2. Yingbo Xie
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  5. Donghui Long
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  6. Licheng Ling
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  7. Wenming Qiao
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Correspondence to Donghui Long or Wenming Qiao.

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Zhang, C., Xie, Y., Wang, J. et al. Effect of graphitic structure on electrochemical ion intercalation into positive and negative electrodes. J Solid State Electrochem 18, 2673–2682 (2014). https://doi.org/10.1007/s10008-014-2527-7

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  • DOI: https://doi.org/10.1007/s10008-014-2527-7

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