Graphene Nanocomposite Materials for Supercapacitor Electrodes: Comparison
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Graphene and related materials (graphene oxide, reduced graphene oxide) as a subclass of carbon materials and their composites have been examined in various functions as materials in supercapacitor electrodes. They have been suggested as active masses for electrodes in electrochemical double-layer capacitors, tested as conducting additives for redox-active materials showing only poor electronic conductivity, and their use as a coating of active materials for corrosion and dissolution protection has been suggested. They have also been examined as a corrosion-protection coating of metallic current collectors; paper-like materials prepared from them have been proposed as mechanical support and as a current collector of supercapacitor electrodes. This entry provides an overview with representative examples. It outlines advantages, challenges, and future directions.

  • graphene
  • reduced graphene oxide
  • nanocomposite
  • supercapacitor
  • electrochemical energy storage
Following the enthusiastic reports about the properties of graphene and later of graphene-related materials like graphene oxide (GO), reduced graphene oxide (rGO) and further materials like crumpled graphene [1[1][2][3][4],2,3,4], suggestions of their use in electrochemistry—wherein carbon in its numerous forms has been a popular material for electrodes or as components of electrode materials has been around for decades—and in particular in devices for electrochemical energy conversion and storage (EES) [5,6][5][6] followed. These suggestions later included their use in supercapacitors [5,7,8,9,10,11,12,13,14,15,16,17,18][5][7][8][9][10][11][12][13][14][15][16][17][18]. As an electrode material in the latter application (as well as in battery applications), materials should meet some general requirements:
  • Large surface area, more specifically electrochemically active surface area (EASA) [19,20][19][20], which will result in large interfacial capacitance;
  • Defined porosity, which translates into accessibility of the EASA, enabling its use in particular at high current densities (the defining property of a supercapacitor) and thus improved capacitance retention [21];
  • High electronic conductivity supporting large current densities without excessive Ohmic losses and associated Joule heat generation (with heating of a supercapacitor known to contribute to ageing [22]);
  • Sufficient chemical, electrochemical, mechanical, and thermal stability affordability.
Further development beyond the pristine materials mentioned above has resulted in 3D materials like graphene foam or monoliths [3,23][3][23] and porous graphene films prepared with a sacrificial template [24,25][24][25]. Nanocarbon materials (or carbon nanostructures) for application in energy conversion and storage including the ones addressed in this entry have been reviewed [26,27,28][26][27][28] for applications in flexible storage devices [29]; for further graphene nanomaterials, see [30]. For other nanostructured materials in energy-related applications, see [31].
Combining graphene and its relatives with other redox-active materials may result in composites having advantageous properties of both constituents, possibly without some of their flaws. These materials and their use in supercapacitors are the focus of this entry. Graphene and its relatives and their use in supercapacitors has been studied extensively and has been reviewed broadly; the respective literature is introduced in the respective sections. Use of these materials beyond supercapacitors is beyond this entry.

References

  1. El Rouby, W.M. A Crumpled graphene: Preparation and applications. RSC Adv. 2015, 5, 66767–66796.
  2. Deng, S.; Berry, V. Wrinkled, rippled and crumpled graphene: An overview of formation mechanism, electronic properties, and applications. Mater. Today 2016, 19, 197–212.
  3. Jiang, L.; Fan, Z. Design of advanced porous graphene materials: From graphene nanomesh to 3D architectures. Nanoscale 2014, 6, 1922–1945.
  4. Mathew, E.E.; Balachandran, M. Crumpled and porous graphene for supercapacitor applications: A short review. Carb. Lett. 2021, 31, 537–555.
  5. Liu, W.R. Graphene-Based Energy Devices. In Graphene-Based Energy Devices; Mohd Yusoff, A.R.b., Ed.; Wiley-VCH: Weinheim, Germany, 2015; pp. 85–122.
  6. Liu, J.; Xue, Y.; Zhang, M.; Dai, L. Graphene-based materials for energy applications. MRS Bull. 2012, 37, 1265–1272.
  7. Liang, M.; Luo, B.; Zhi, L. Application of graphene and graphene-based materials in clean energy-related devices. Int. J. Energy Res. 2009, 33, 1161–1170.
  8. Huang, Y.; Liang, J.; Chen, Y. An overview of the applications of graphene-based materials in supercapacitors. Small 2012, 8, 1805–1834.
  9. Ghosh, A.; Lee, Y.H. Carbon-based electrochemical capacitors. ChemSusChem 2012, 5, 480–499.
  10. Choi, H.J.; Jung, S.M.; Seo, J.M.; Chang, D.W.; Dai, L.; Baek, J.B. Graphene for energy conversion and storage in fuel cells and supercapacitors. Nano Energy 2012, 1, 534–551.
  11. Minisha, S.; Vedhi, C.; Rajakani, P. Review-Methods of Graphene Synthesis and Graphene-Based Electrode Material for Supercapacitor Applications. ECS J. Solid State Sci. Technol. 2022, 11, 111002.
  12. Aleksandrzak, M.; Mijowska, E. Graphene and Its Derivatives for Energy Storage. In Graphene Materials: Fundamentals and Emerging Applications; Tiwari, A., Syväjärvi, M., Eds.; Scrivener Publishing: Salem, MA, USA; WILEY: Hoboken, NJ, USA, 2015; pp. 191–224.
  13. Tan, Y.B.; Lee, J.M. Graphene for supercapacitor applications. J. Mater. Chem. A 2013, 1, 14814–14843.
  14. Ramesha, G.K.; Sampath, S. Graphene and graphene-oxide-based materials for electrochemical energy systems. In Graphene; Rao, C.N.R., Sood, A.K., Eds.; Wiley-VCH: Weinheim, Germany, 2013; pp. 269–301.
  15. Hou, J.; Shao, Y.; Ellis, M.W.; Moore, R.B.; Yi, B. Graphene-based electrochemical energy conversion and storage: Fuel cells, supercapacitors and lithium ion batteries. Phys. Chem. Chem. Phys. 2011, 13, 15384–15402.
  16. Sun, Y.; Wu, Q.; Shi, G. Graphene based new energy materials. Energy Environ. Sci. 2011, 4, 1113–1132.
  17. Tiwari, A.; Uzun, L. (Eds.) Advanced Functional Materials; Scrivener Publishing: Beverly, MA, USA, 2015.
  18. Bich, H.N.; Van, H.N. Promising applications of graphene and graphene-based nanostructures. Adv. Nat. Sci. Nanosci. Nanotechnol. 2016, 7, 023002.
  19. Xie, X.; Holze, R. Electrode Kinetic Data: Geometric vs. Real Surface Area. Batteries 2022, 8, 146.
  20. Xie, X.; Holze, R. Meaning and Determination of Electrode Surface Area. Available online: https://encyclopedia.pub/entry/41569 (accessed on 11 September 2023).
  21. Ge, Y.; Liu, Z.; Wu, Y.; Holze, R. On the utilization of supercapacitor electrode materials. Electrochim. Acta 2021, 366, 137390.
  22. Chen, X.; Wu, Y.; Holze, R. Ag(e)ing and Degradation of Supercapacitors: Causes, Mechanisms, Models and Countermeasures. Molecules 2023, 28, 5028.
  23. Velasco, A.; Ryu, Y.K.; Boscá, A.; Ladrón-De-Guevara, A.; Hunt, E.; Zuo, J.; Pedrós, J.; Calle, F.; Martinez, J. Recent trends in graphene supercapacitors: From large area to microsupercapacitors. Sustain. Energy Fuels 2021, 5, 1235–1254.
  24. Liu, M.; Wei, F.; Yang, X.; Dong, S.; Li, Y.; He, X. Synthesis of porous graphene-like carbon materials for high-performance supercapacitors from petroleum pitch using nano-CaCO3 as a template. New Carbon Mater. 2018, 33, 316–323.
  25. Meng, Y.; Wang, K.; Zhang, Y.; Wei, Z. Hierarchical Porous Graphene/Polyaniline Composite Film with Superior Rate Performance for Flexible Supercapacitors. Adv. Mater. 2013, 25, 6985–6990.
  26. Chen, X.; Paul, R.; Dai, L. Carbon-based supercapacitors for efficient energy storage. Nat. Sci. Rev. 2017, 4, 453–489.
  27. Jiang, H.; Lee, P.S.; Li, C. 3D carbon based nanostructures for advanced supercapacitors. Energy Environ. Sci. 2013, 6, 41–53.
  28. Dai, L.; Chang, D.W.; Baek, J.B.; Lu, W. Carbon nanomaterials for advanced energy conversion and storage. Small 2012, 8, 1130–1166.
  29. Cheng, Y.; Liu, J. Carbon nanomaterials for flexible energy storage. Mater. Res. Lett. 2013, 1, 175–192.
  30. Liu, F.; Xue, D. Advanced graphene nanomaterials for electrochemical energy storage. Mater. Res. Innov. 2015, 19, 7–19.
  31. Arico, A.S.; Bruce, P.; Scrosati, B.; Tarascon, J.M.; van Schalkwijk, W. Nanostructured materials for advanced energy conversion and storage devices. Nat. Mater. 2005, 4, 366–377.
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