Carbon Nanotube and Graphene-Based Supercapacitors: 

Rationale, Status, and Prospects 

by Matthew H. Ervin 

ARL-TR-5283 August 2010 

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ARL-TR-5283 August 2010 

Carbon Nanotube and Graphene Based Supercapacitors: 

Rationale, Status, and Prospects 

Matthew H. Ervin 

Sensors and Electron Devices Directorate, ARL 

Approved for public release; distribution unlimited. 
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Carbon Nanotube and Graphene Based Supercapacitors: Rationale, Status, and 

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14. ABSTRACT 

In a supercapacitor, the surface area of the electrodes accessible to the solvated electrolyte ions determines the capacitance;

therefore, carbon materials with improved surface area may increase the energy density of supercapacitors. Two materials 

being studied for this are carbon nanotubes (CNTs) and graphene. Since all of their atoms are surface atoms, extremely large 

surface areas per mass may be obtainable. CNTs also have inherently high conductivity, which should increase the power 

density of these capacitors. To date, CNT supercapacitors have only matched state-of-the-art activated carbon supercapacitor 

performance. Factors limiting CNT supercapacitors are explored and future prospects are considered. 

15. SUBJECT TERMS

Supercapacitor, electrochemical capacitor, carbon nanotube, graphene 

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iii 

Contents 

List of Tables iv

1. Background 1

2. Rationale for CNTs/Graphene 2

3. CNT/Graphene Processing 3

4. Capacitance Limits 5

5. Capacitor Evaluation 6

6. Conclusions and Opportunities 7

7. References 8

List of Symbols, Abbreviations, and Acronyms 10 

Distribution List 11 
iv 

List of Tables 

Table 1. Examples of solution processed CNT/graphene electrodes. .............................................4
1 

1. Background 

Portable power sources, such as batteries, are a critical part of a Soldier’s equipment. Therefore, 

advances in portable power production and storage are of great interest to the Army. 

Supercapacitors have several advantages over conventional batteries, including higher specific 

power (~2 orders of magnitude higher than batteries and fuel cells), higher cycle life (able to 

withstand millions of charge/discharge cycles), rapid charge/discharge times (seconds to 

minutes), high efficiencies (up to 98%), and unaltered performance in extreme heat and cold (1). 

Their quick-charge capability would mean they could be charged in a few minutes before a 

patrol. As it is, Soldiers are replacing their batteries before each patrol to guard against 

equipment failure in the field. This represents a significant logistical burden in supplying and 

disposing of batteries. Unfortunately, current state-of-the-art supercapacitors lack the energy 

density to make them competitive with conventional batteries for most portable power 

applications. 

In the area of electrical energy storage, capacitors compete with batteries and fuel cells. 

(Capacitors have a wide variety of other applications in addition to energy storage, such as 

providing pulse power and signal filtering, and creating resonant circuits.) Batteries and 

capacitors are similar in many ways, but they store energy using two different mechanisms. 

Batteries store energy via reduction and oxidation (redox) reactions at their electrodes, whereas 

capacitors store energy in an electric field across a dielectric. As a result, batteries and 

capacitors have significantly different characteristics. Batteries excel at providing high energy 

densities at low power, while conventional capacitors have high power densities but low energy 

density. A special type of capacitor, a supercapacitor (also called an ultracapacitor or 

electrochemical double layer capacitor), has high power density along with moderate energy 

density. 

A traditional capacitor consists of two metal plates separated by a thin dielectric. The larger the 

overlapping electrode surface area and the thinner the dielectric, the higher the capacitance. An 

electrolytic capacitor has a metal electrode covered with a dielectric, with the second electrode 

being a liquid electrolyte. Again, the overlapping surface area between the dielectric-coated 

electrode and the liquid electrode, along with the dielectric thickness, combine to determine the 

capacitance. 

A supercapacitor consists of two solid electrodes in contact with a liquid electrolyte without any 

dielectrics (although there is an electrolyte permeable electrode separator to prevent shorting of 

the electrodes). Supercapacitors store charge by inducing the adsorption of ions onto the 

electrodes using an electric field. When a potential is applied across the electrodes, the positive 

ions in the electrolyte will adsorb onto the negative electrode and the negative ions onto the 

positive electrode. Since there is no dielectric on the electrodes, the applied biases must remain 
2 

low enough that charge transfer between the ions and the electrodes, as well as electrochemical 

breakdown of the electrolyte solvent, do not occur. This limits the voltage rating on individual 

supercapacitor cells to about 1.2 V when using aqueous electrolytes, and 3.5 V when using 

organic electrolytes. 

2. Rationale for CNTs/Graphene 

Supercapacitors were first commercialized in 1978 by NEC Corporation. In a supercapacitor, 

large capacitances are achieved by using electrodes with very large surface areas. Commercial 

supercapacitors use carbon electrodes made from highly porous “activated” carbon (typically 

derived from coconut shells) and a binder material attached to a highly conductive current 

collector. Carbide-, fiber-, and sugar-derived activated carbons are under development to 

improve upon the performance of activated carbon. Carbon electrodes are desirable due to their 

favorable physical and chemical properties. They are conductive, can be made with high surface 

area, have good corrosion resistance, have good thermal stability, and are made using 

inexpensive materials (1). Since the surface area of the electrodes accessible to the solvated 

electrolyte ions determines the capacitance, carbon materials with improved surface area may 

increase the capacity of supercapacitors. Two materials being studied for this are carbon 

nanotubes (CNTs) and graphene. CNTs are single or multiple atomic layers of graphite that 

curve back on themselves to form tubes, while graphene is a single atomic layer of graphite. 

CNTs are potential candidates since, in the case of single wall nanotubes (SWCNTs), all of the 

carbon atoms are surface atoms; consequently, extremely large surface areas may be obtainable 

if the CNTs can be assembled in a manner that maximizes the surface area by minimizing CNT 

bundling and optimizing the porosity of the CNT electrode. The outside of SWCNTs have a 

theoretical surface area of 1320 m2

/g, though the scientific literature typically reports surface 

areas of <450 m2

/g based on nitrogen absorption studies. This indicates that there is significant 

potential for CNT surface area improvement by optimizing the morphology of the CNT film. 

CNTs also have inherently high conductivity, and their fibrous nature may eliminate the need for 

an inert binder so that the resulting electrode may have improved conductivity. This will 

contribute to a low equivalent series resistance and, therefore, increased power output. On the 

downside, CNT growth produces a mixture of 2/3 semiconducting and 1/3 metallic SWCNTs, 

with the semiconducting tubes expected to contribute little to the capacitance due to their low 

density of states (2). (Our own experiments have yet to demonstrate this.) If it is true that 

semiconducting tubes do not contribute significantly to capacitance, that would also mean that 

graphene nanoribbons formed by unzipping CNTs (3), as was originally proposed, would not be 

a viable approach since all graphene nanoribbons are semiconducting if they are narrow enough. 

This would not be a problem with larger graphene platelettes. Multiwall CNTs (MWCNTs) tend 

to be metallic as chances are good that at least one of the nested shells is metallic, but the 
3 

semiconducting shells may still be dead weight. Cost is also a significant issue, as SWCNTs can 

cost ~$100,000/kg, and MWCNTs can cost ~$5, 000/kg, while activated carbon costs just 

~$15/kg. 

Graphene is an even more recent entry into the supercapacitor arena. Graphene, again, is 

composed of all surface atoms, but now both sides of the layer are accessible, giving it a 

theoretical surface area of 2640 m2

/g. While activated carbon is sometimes measured to have 

similar surface area, this is almost certainly overstated by the measurement technique; in any 

case, it is clear that all of the measured surface area is not accessible to the electrolyte ions. A 

significant advantage of graphene over CNTs is that there are a number of methods—e.g., 

chemical exfoliation—for producing it from graphite. Indeed, commercial scale production of 

graphene in ton quantities is underway, which should result in much more competitive prices 

than for CNTs. While graphene has potentially more surface area, its morphology may make it 

more difficult to produce a porous electrode, as the graphene sheets are likely to stack on top of 

one another without intervening pore volume for the electrolyte. 

3. CNT/Graphene Processing 

Both CNT and graphene materials are frequently processed as suspensions/solutions. In order to 

get stable dispersions in a solvent, the CNTs or graphene are either chemically functionalized 

and/or dispersed with the aid of a surfactant. Both approaches have their drawbacks. Chemical 

functionalization, for instance, by adding carboxylic acid groups to the material with the aid of a 

strong acid, can make the material more soluble in water. However, the addition of these 

functional groups introduces defects in the lattice structure of the material that can decrease its 

conductivity. Such functional groups can also represent red-ox groups, which can incorporate 

pseudocapacitance in the capacitor that may or may not be desirable. (Pseudocapacitance is 

(dis)charging resulting from redox reactions like a battery, but which occur at a potential 

dependent rate so that they behave like a capacitance.) While the presence of pseudocapacitance 

can increase the capacitance, the eventual decomposition of functional groups and impurities can 

result in gas liberation—e.g., carboxylic acid groups converting to carbon dioxide (CO2)—which 

can rupture the device package. Pseudocapacitance derived from incorporated nanoparticles or 

thin films of selected materials, such as manganese or ruthenium dioxide (MnO2 or RuO2), can 

increase the total capacitance by several times. 

Surfactants can be used in place of functionalization to help solubilize CNTs or graphene, but 

since they are generally nonconductive, themselves, they will impede charge transfer between 

the nanomaterials. Therefore, further processing may be required to clean them, which may 

remove the CNTs/graphene from the substrate or alter the electrode morphology (4).
4 

These solution-based processing issues can be avoided by growing the CNTs or graphene 

directly on the current collector. In the case of CNTs, this has been done using chemical vapor 

deposition (CVD) by several groups (5). Growing vertical arrays of CNTs is attractive, as the 

vertical CNTs have, in effect, vertically aligned pores that allow for efficient ion transport into 

and out of the electrode. On the other hand, it may be difficult to optimize the density (porosity) 

of the electrode, and the process has limited throughput. As CVD is a high temperature >700 °C 

process, there are also limits on the current collector materials used, and there is difficulty 

integrating the process for on-chip or other specialized applications. For these reasons, and 

increased options for manufacturing, solution-based processing is likely to be a more costeffective and flexible option. Many solution-based processing approaches have been 

demonstrated with some recent examples given in table 1. The solution-based processing 

approaches in table 1 have demonstrated 23–200 F/g, although the higher values likely include 

pseudocapacitive contributions. For comparison, state-of-the-art activated carbons yield specific 

capacitances of up to 120 F/g. A review of the scientific literature has shown that commercially 

available activated carbon supercapacitors using aqueous electrolyte exhibit a specific 

capacitance of 33 F/g, a specific energy of 13 Wh/kg, and a specific power of 0.58 kW/kg (6). 

Table 1. Examples of solution processed CNT/graphene electrodes. 

Deposition 

method 

CNT solution F/g Comments Reference 

Spray Deposition SWCNT 38 CNTs not functionalized 7 

Spray Deposition SWCNT-COOH 155 Functionalization results in clear 

redox pseudocapacitance 

7

Spray Deposition MWCNT 23 CNTs not functionalized 7

Spray Deposition MWCNT-COOH 77 Functionalization results in clear 

redox pseudocapacitance 

7

Spray Deposition SWCNT 90–120 CNTs possibly functionalized during 

purification 

8 

Layer by Layer MWCNT-COOH 

MWCNT-NH2 

150 Pseudocapacitance contribution 9 

Filtration DWCNT 67 DNA dispersed double walled CNTs 10 

Filtration DWCNT 32 Double walled CNTs 11 

Electrospray MWCNT-COOH 108 Pseudocapacitance contribution 12 

Meyer Rod - 

Adsorb on Paper 

SWCNT 200 Measurements indicate at least some 

pseudocapaitance 

4 

Freeze Dry graphene 120 200C anneal of graphene oxide may 

not remove all oxide functional 

groups 

13 
5 

4. Capacitance Limits 

What is the theoretical specific capacitance for SWCNTs? The theoretical limits are determined 

by the surface area per gram, which is 1320 m2

/g for SWCNTs, and the size of the solvated ions 

of the electrolyte, which combine to determine how many ions can adsorb on a gram of 

SWCNTs. The capacitance achievable per electrode area for potassium hydroxide and sulfuric 

acid (KOH, H2SO4), and common organic electrolytes are 74, 42, and ~20 μF/cm2 (valid at ~1V), 

respectively. (At very high electrolyte concentrations, these numbers can be increased when the 

effective ion size is reduced by preventing the outer salvation spheres with a shortage of solvent.) 

This yields a theoretical specific capacitance limit of 977 F/g for SWCNTs; this amount is 

double for graphene. If one assumes the usual ratio of 1/3 metallic SWCNTs, and that the 

semiconducting tubes do not participate, this number is reduced to 325 F/g for SWCNTs. 

It should be noted that activated carbon does not come close to its maximum specific 

capacitance, calculated using nitrogen absorption surface area measurements. This is probably 

due to errors in the measurement methodology, as well as to the fact that surface area available to 

nitrogen molecules is not all available to the larger solvated electrolyte ions (14). Perhaps a 

more important restriction is that as ions are electrostatically drawn into the activated carbon 

pores, they naturally adsorb at the first available site. Consequently, the mouth of the pore is 

blocked by the first ions to arrive, leaving the rest of the pore area to be unused (15). Since 

CNTs and graphene have their surface area all on the outside, it should be possible to tailor their 

morphology to more effectively use the surface area. 

As it turns out, there may be another reason CNTs, graphene, and activated carbon do not attain 

the theoretical specific capacitances calculated. Single-layer graphene or SWCNTs may not be 

able to polarize a full monolayer of electrolyte ions due to an insufficient number of carriers in 

one atomic layer. This implies that there are not enough carriers in a CNT or graphene sheet to 

completely screen the field from the adsorbed ions so that the field penetrates through to the 

other side, diminishing the number of ions that can adsorb there (16, 17). Alternately, one can 

think of the electrode capacitance being a combination of interfacial capacitance (the adsorbed 

ions/double layer) and the quantum capacitance of the CNT/graphene (18, 19). Since these 

capacitances combine as capacitors in series, the smaller capacitance (in this case, the quantum 

capacitance) will dominate so that the calculated interfacial capacitance will not be achieved. If 

one were to assume that it takes two CNT shells to screen the field from ions adsorbed on the 

outside, then the maximum specific capacitance would be achieved for double-wall CNTs with 

490F/g (in KOH) with all shells metallic, or 160 F/g for mixed semiconducting and metallic 

shells (if the semiconducting shells do not contribute). Graphene would then need four layers to 

support the full capacitance available with its surface area, with a similar reduction in achievable 

specific capacitance. More work is required to determine if this is a serious limitation. 
6 

5. Capacitor Evaluation 

When characterizing capacitors, one needs to be careful to distinguish between true capacitance 

and any redox contributions. In table 1, the metric of specific capacitance has been used as a 

measure of how much useable surface area is being obtained. When pseudocapacitance is 

present, it can then be difficult to determine how much capacitance is due to true capacitance 

resulting from the large surface area versus that due to redox-based pseudocapacitance. 

However, even without pseudocapacitance, it can be difficult to compare results. Factors such as 

measurement methodology (cyclic voltametry versus constant current measurements), 

measurement parameters, and the electrolytes used can contribute to significant differences in 

measured capacitances. The measurements must be made under realistic conditions so that 

measured capacitances will reflect practically usable values. A review of the literature by Istvan 

has revealed that changing the CV scan rate from 5 to 20 mV/s, or the galvanostatic 

charge/discharge current from 10 to 200 mA/g, will reduce the measured capacitance by 20% 

(15). Standard test conditions of 20 mV/s and 200 mA/g or higher are, therefore, recommended. 

Another important testing factor is that the device must be cycled many times before testing in 

order to exhaust any irreversible redox contributions to the capacitance due to impurities that 

would exaggerate the measured capacitance. 

To this point in the discussion, I have focused on the specific capacitance (F/g) figure of merit, 

which reflects how effectively the electrode material is being used. Other important figures of 

merit include rated voltage (V), capacitance (F), resistance (Ω), time constant (s), specific energy 

(Wh/kg), and specific power (W/kg), as well as volumetric measures of capacitance, power, and 

energy. Obviously, many of these factors are interrelated. In research papers, the specific 

capacitance is usually calculated using the mass of the carbon (e.g., CNTs) only, since it reflects 

how good the carbon electrode morphology is, and since the electrodes are frequently not 

packaged into devices. However, in a commercial device, the farads per gram specification will 

generally be calculated using the entire mass of the capacitor because, for the final application, it 

is the entire mass of the capacitor that is relevant. In a packaged device, it is the capacitance, 

energy, and power available per packed device weight or volume that will be most important. To 

get an idea of where supercapacitor technology stands, it is useful to look at a survey of activated 

carbon supercapacitors under industrial development, which have been characterized in Andrew 

Burke’s lab at the University of California (UC)-Davis (20). Burke has found that the current 

crop of supercapacitors under development have specific capacitances of 3 to 10 F/g (total device 

weight), specific energies of 2.3 to 12 Wh/kg, specific powers of 390–5700 W/kg, and 

volumetric capacitances of 3–15 F/cc. These are important specifications to keep in mind while 

developing CNT/graphene supercapacitors. 
7 

6. Conclusions and Opportunities 

CNTs have yet to convincingly exceed the specific capacitance of activated carbon in the 

absence of pseudocapacitance, but even if they do not, CNTs/graphene may still yield 

improvements in power due to increased electrode conductance. There may also be important 

supercapacitor improvements due to the mechanical properties of CNTs/graphene. For instance, 

CNTs/graphene may lend themselves to flexible, conformal, or integrated supercapacitors that 

would be useful for applications where there is little available space. It would also be desirable 

to develop supercapacitors that could be used as structural elements. 

Much recent work on supercapacitors has focused on increasing their energy density so that they 

can compete with batteries. This may take the form of incorporating increasing amounts of 

pseudocapacitance. Similarly, a lot of effort has gone into increasing battery power density, 

which may be achieved by reducing the discharge depth at the expense of energy density. In 

each case, a technology’s strength is being compromised in order to shore up a weakness. In the 

end, it is probably more logical to develop a hybrid system that couples a supercapacitor to a 

battery or other energy source. The battery slowly charges the supercapacitor, which then 

supplies the peak power loads of the system. The supercapacitor could also level the load from 

intermittent or regenerative power recovery systems. In this approach, the supercapacitor could 

extend the power load the battery could support and extend the battery’s lifetime by reducing the 

number and depth of charge/discharge cycles. Such a hybrid could capture the best performance 

of each technology. 
8 

7. References 

1. Pandolfo, A. G.; Hollenkamp, A. F. J. Power Sources 2006, 157, 11–27. 

2. Shylau, A. A.; Klos, J. W.; Zozoulenko, I. V. Phys. Rev. B 2009, 80, 205402. 

3. Kosynkin, D. V.; Higginbotham, A. L.; Sinitskii, A.; Lomeda, J. R.; Dimiev, A.; Price, B. K.; 

Tour, J. M. Nature Letts. 2009, 458, 872–876. 

4. Hu, L.; Choi, J. W.; Yang, Y.; Jeong, S.; La Mantia, F.; Cui, L.-F.; Cui, Y. Proc. Nat. Acad. 

Sci. 2009, 106, 21490–21494. 

5. Jiang, Y. Q.; Zhou, Q.; Lin, L. 2009 IEEE 22nd International Conference on Micro Electro 

Mechanical Systems, Sorrento Italy, 2009, pp. 587–590. 

6. Obreja, V.V.N. Physica E. 2008, 40, 2596–2605. 

7. Zhao, X.; Chu, B.T.T.; Ballesteros, B.; Wang, W.; Johnston, C.; Sykes, J. M.; Grant, P. S. 

Nanotech. 2009, 20, 065605. 

8. Kaempgen, M.; Chan, C. K.; Ma, J.; Cui, Y.; Gruner, G. Nano Lett 2009, 9, 1872–1876. 

9. Lee, S. W.; Kim, B.-S.; Chen, S.; Shao-Horn, Y.; Hammond, P. T. J. Amer. Chem. Soc.

2009, 131, 671–679. 

10. Cooper; et al. Appl. Phys. Lett. 2009, 95, 233104. 

11. Chou, S.-L.; Wanga, J.-Z.; Chew, S.-Y.; Liu, H.-K.; Dou, S.-X. Electrochem. Comm. 2008, 

10, 1724–1727. 

12. Kim, J. H.; Nam, K.-W.; Ma, S. B.; Kim, K. B. Carbon 2006, 44, 1963–1968. 

13. Wang, J.; Ellsworth, M. W. Electrochem. Soc. Trans. 2009, 19, 241–247. 

14. Liu, C.; Cheng, H. M. J. Phys. D: Appl Phys. 38, R231–R252 (2005). 

15. Isvan, R. The 19th Int’l Seminar on Double Layer Capacitors and Hybrid Energy Storage 

Devices, Deerfield Beach, FL, 7–9 Dec 2009. 

16. Barbieri, O.; Han, M.; Herzog, A.; Kotz, R. Carbon 2005, 43, 1303–1310. 

17. Hahn, M.; Baertschi, M.; Barbieri, O.; Sauter, J.-C.; Kotz, R.; Gallay, R. Electrochem. and 

Solid State Lett. 2004, 7, A33–A36. 

18. Xia, J.; Chen, F.; Li, J.; Tao, N. Nature Nanotech. 2009, 4, 505–509. 
9 

19. Wang, D.-W.; Li, F.; Wu, Z.-S.; Ren, W.; Cheng, H.-M. Electrochem. Comm. 2009, 11, 

1729–1732. 

20. Burke, A.; Miller, M. The 19th Int’l Seminar on Double Layer Capacitors and Hybrid 

Energy Storage Devices, Deerfield Beach, FL, 7–9 Dec 2009. 
10 

List of Symbols, Abbreviations, and Acronyms 

CNT carbon nanotube 

CO2 carbon dioxide 

CVD chemical vapor deposition 

DWCNT double wall carbon nanotube 

F farads (capacitance) 

F/g farads per gram (specific capacitance) 

H2SO4 sulfuric acid 

KOH potassium hydroxide 

MWCNT multi-wall carbon nanotube 

MWCNT-COOH carboxylic acid functionalized multi-wall carbon nanotube 

MWCNT-NH2 amine functionalized multi-wall carbon nanotube 

MNO2 manganese dioxide 

RuO2 ruthenium dioxide 

S seconds 

SWCNT single wall carbon nanotube 

SWCNT-COOH carboxylic acid functionalized single wall carbon nanotube 

V volts 

Ω Ohms (resistance) 

W/kg Watts per kilogram (specific power) 

Wh/kg Watt hours per kilogram (specific energy) 
11 

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