Carbon 40 (2002) 667–674

Influence of oxygen treatment on electric double-layer

capacitance of activated carbon fabrics
Chien-To Hsieh, Hsisheng Teng*
Department of Chemical Engineering, National Cheng Kung University, Tainan 70101, Taiwan
Received 20 December 2000; accepted 30 April 2001

Abstract

Oxygen treatment at 2508C on polyacrylonitrile-based activated carbon fabric was conducted to explore the influence of
carbon–oxygen complexes on the performance of capacitors fabricated with the carbon fabric. Surface analysis showed that
most of the oxygen functional groups created from the oxygen treatment were the carbonyl or quinone type. The
performance of the capacitors was tested in 1 M H 2 SO 4 , using potential sweep cyclic voltammetry and constant current
charge–discharge cycling. It was found that the Faradaic current, the contributor of pseudocapacitance, increased
significantly with the extent of oxygen treatment, while the increase in the double-layer capacitance was minor. Due to the
treatment the overall specific capacitance showed an increase up to 25% (e.g., from 120 to 150 F g 21 at a current density of
0.5 mA cm 22 ). However, the distributed capacitance effect, the inner resistance and the leakage current were found to
increase with the extent of oxidation. It is suggested that due to the local changes of charge density and the increase in redox
activity the presence of the carbonyl- or quinone-type functional groups may induce double-layer formation, Faradaic
current, surface polarity, and electrolyte decomposition.  2002 Elsevier Science Ltd. All rights reserved.

Keywords: A. Activated carbon; B. Oxidation; C. Electrochemical analysis; D. Electrochemical properties, Functional groups

1. Introduction capacitors [3–7]. The effects of the specific surface area,

Carbons of different forms have been extensively used
in a variety of electrochemical systems [1], such as
batteries and electric double-layer capacitors (EDLCs).
Previous studies have pointed out that carbon fibers from
polyacrylonitrile (PAN) precursor provide good electrical
properties and high strength [1,2]. Recently, interest in
PAN-based activated carbon fabrics for the use as porous
electrodes in EDLCs has emerged. One of the advantages
of carbon fabrics over fibers or powders is that there is no
binding material required in the fabrication of electrodes.
The cost of binding materials, such as polytetrafluoro-
ethylene or polyvinylidenefluoride, for electrode prepara-
tion is usually high, and the binders may block some
entrances of the pores in the porous carbons, hence
resulting in diminishment of double-layer capacitance.
It is well known that the pore structures of carbon
electrodes affect the performance of the resulting
*Corresponding author. Tel.: 1886-6-2385-371; fax: 1886-6-
2344-496.
E-mail address: hteng@mail.ncku.edu.tw (H. Teng).
as well as the pore size distribution, of the carbon
electrodes has been discussed. Apart from the physical
structures, the chemical characteristics, such as the dis-
tribution of heteroatoms on carbon surface, would also
influence the capacitor performance. The carbon–oxygen
complexes, i.e., the oxygen functional groups, in carbons
have been reported to be the important surface groups
affecting the wettability, chemical reactivity, and electrical
properties [1,8,9]. How these complexes can affect the
performance of the resulting EDLCs was rarely reported in
the literature.
Oxygen functional groups can be formed on carbons by
treatments such as electrochemical oxidation [2], cold
plasma treatment [10], chemical oxidation in HNO 3 or
H 2 SO 4 solutions [9,11], and gaseous oxidation with oxi-
dizing gases [12]. In examining the effects of oxygen
functional groups, employing gaseous oxidation to create
the functional groups has the advantages such as con-
venience and no significant impact on physical characteris-
tics of the carbons. Without the intrusion of pore structure
change, the effects of oxygen functional groups can be
exclusively discussed.

0008-6223 / 02 / $ – see front matter  2002 Elsevier Science Ltd. All rights reserved.
PII: S0008-6223( 01 )00182-8
668 C.-T. Hsieh, H. Teng / Carbon 40 (2002) 667 – 674
Within the above scope the performance of EDLCs
fabricated using oxidized PAN-based carbon fabrics was
examined. Gaseous oxidation using oxygen as the oxi-
dizing agent was employed in the present work. The
chemical composition of the resulting carbon–oxygen
complexes was analyzed, in the attempt to elucidate the
effects of different oxygen functional groups during the
course of double layer formation at the electrolyte–carbon
interface.
2. Experimental
2.1. Oxidation of activated carbon fabrics
PAN-based activated carbon fabric supplied by Taiwan
Carbon Technology, Taiwan, was used to fabricate the
electrodes of EDLCs. The fabric has a thickness of 0.4–0.6
mm. The diameter of the carbon fibers in the fabric is ca.
15 mm. Oxidation was carried out with thermal treatment
at 2508C under an oxygen atmosphere. Because of the
negligible extent of carbon gasification at this treatment
temperature, weight gain due to oxygen chemisorption,
rather than weight loss, was observed in the oxidation. The
treatment was conducted for different lengths of time to
prepare samples containing different populations of oxygen
functional groups on the surface.
2.2. Characterization of carbon fabrics
Physical characteristics of the carbon fabrics were
determined by N 2 adsorption at 21968C, using an auto-
mated adsorption apparatus (Micromeritics, ASAP 2010).
Surface areas and micropore volumes of the samples were
evaluated with the application of the BET and Dubinin–
Radushkevich (D–R) equations, respectively. The amount
of N 2 adsorbed at relative pressure near unity was em-
ployed to determine the total pore volume, which corre-
sponds to the sum of the micropore and mesopore volumes
[13]. The average pore diameter was estimated according
to the surface area and total pore volume, assuming that
the pores are parallel and cylindrical.
A temperature programmed desorption (TPD) technique
was employed to analyze the population of carbon–oxygen
complexes on the carbon fabrics. The experiments were
Table 1
Physical characteristics of the carbon fabrics used as the electrodes for electrochemical measurements
Carbon Oxidation BET surface
type time (h) area (m 2 g 21 )
CF 0 1290
CFO1 0.5 1280
CFO2 1 1270
CFO3 6 1190
carried out under a helium flow, by heating 0.05 g of
sample from room temperature to 9008C with a linear rate
of 308C min 21 . The evolution of CO and CO 2 during TPD
was continuously monitored with non-dispersive infrared
analyzers.
The chemical composition of the oxygen functional
groups was also studied by X-ray photoelectron spec-
troscopy (XPS). The XP spectra were recorded with a
Fisons VG ESCA210 spectrometer and Mg K a radiation.
The spectra were smoothed and a non-linear background
was subtracted. The deconvolution of the spectra was
performed using a non-linear least-squares fitting program
with a symmetric Gaussian function. The surface com-
position of the samples was calculated with C 1s and O 1s
peaks [14] and appropriate sensitivity factors.
2.3. Electrochemical measurements
Two electrode cells were used to examine the electro-
chemical performance of the carbon fabrics. The electrodes
consisted of 2 cm 2 carbon fabrics and stainless steel foils
serving as the current collector. The cells were constructed
with two facing carbon electrodes, sandwiching a piece of
filter paper as separator. All electrochemical measurements
were performed at ambient temperature, by soaking the
cells in an electrolyte solution of 1 M H 2 SO 4 . Cyclic
voltammetric measurements of the cells were made in the
potential range of 20.6 to 0.6 V applied between the two
electrodes. The potential scan rate ranged from 0.5 to 5 mV
s 21 . The capacitance of the cells was measured by
charging the capacitors to 0.6 V, followed by discharging
to 0 V at constant currents of 0.5, 1, 2, and 5 mA. The
leakage current test was performed at a floating potential
of 0.6 V for more than 12 h.
3. Results and discussion
3.1. Surface characteristics of carbon fabrics
The physical characteristics of the carbon fabrics are
given in Table 1. The original carbon fabric is designated
as CF and the oxidized fabrics are designated as CFO1,
CFO2 and CFO3, which were derived from oxidizing CF
for 0.5, 1 and 6 h, respectively. The pore size distribution
Pore volume Pore size distribution Average pore
(cm 3 g 21 ) diameter (nm)
Micro (%) Meso (%)
0.62 100 0 1.93
0.61 100 0 1.92
0.61 100 0 1.92
0.57 100 0 1.92
 C.-T. Hsieh, H. Teng / Carbon 40 (2002) 667 – 674
shows that these carbons are highly microporous. The
surface area and pore volume decrease slightly with the
extent of oxygen treatment. This indicates that introduction
of oxygen functional groups in micropores has hindered
the access of N 2 to some of these pores. Although physical
characteristics of carbons, including the degree of order
[15] and the exposed area [6], have been shown to affect
the performance of the resulting capacitors, their influence
will be considered to be minor in the present work since
the degree of order cannot be altered at 2508C and the
changes in surface area and pore size distribution caused
by the oxygen treatment are, as a matter of fact, not
notable.
The population of oxygen functional groups built up
during the oxygen treatment has been evaluated using
TPD. Past studies have reported that during the course of
TPD oxygen functional groups such as carboxyl, anhydride
and lactone groups would evolve as CO 2 while hydroxyl,
carbonyl and quinone groups would evolve as CO
[1,16,17]. The accumulated amounts of CO and CO 2
evolution during TPD are given in Table 2. The results
show that the amount of CO 2 evolved from these carbon
fabrics increases slightly with the extent of treatment,
while the amount of CO evolved was significantly en-
hanced upon oxidation. The increase in total oxygen
evolution from the fabrics with the extent of oxidation can
be attributed mainly to the formation of the CO-desorbing
complexes, which are essentially basic in chemical nature
[8].
XPS was employed for further analysis of the com-
position of the oxygen functionalities on the carbon
fabrics. The C 1s and O 1s peaks of the scan spectra have
binding energies of ca. 284.6 and 533.5 eV, respectively.
Quantitative analysis was carried out to determine the
surface C and O concentrations, and the (O 1s) /(C 1s)
atomic ratios are listed in Table 3, showing that the ratio
increases with the extent of oxidation. The trend of (O
1s) /(C 1s) varying with the oxidation level is similar to
that of total oxygen evolution in TPD shown in Table 2.
The broad C 1s peak ranging from 280 to 292 eV in the XP
spectra may comprise peaks contributed by several carbon-
based functional groups that have different binding ener-
gies. These binding energy peaks have been identified as C
Table 2
Accumulated amounts and percentages of CO and CO 2 evolution
from the carbon fabrics during temperature programmed desorp-
tion
Carbon CO evolution CO 2 evolution Total O evolution
type 21 21 (mmol g 21 )
mmol g % mmol g %
CF 0.23 58 0.17 42 0.57
CFO1 0.41 68 0.19 32 0.79
CFO2 0.58 74 0.20 26 0.98
CFO3 0.81 76 0.25 24 1.31
669
Table 3
(O 1s) /(C 1s) atomic ratio and distribution of oxygen functional
groups of carbon fabrics determined from deconvolution of XP C
1s spectra
Carbon (O 1s) /(C 1s) Functional group distribution
type
C–O (%) C=O (%) O–C=O (%)
CF 0.064 48 14 38
CFO1 0.086 40 28 32
CFO2 0.11 30 41 29
CFO3 0.13 24 51 25
or C–H at 284.6 eV, C–O at 286.7 eV, C=O at 288.4 eV and
O–C=O at 289.7 eV [18–20]. The C 1s peak of each
carbon can be deconvoluted using a peak synthesis pro-
cedure in which Gaussian peak shape was assumed to fit
each component with a fixed binding energy and an
average full width half maximum value of 2.0 eV. The
distribution of oxygen-containing groups of each carbon
was thus determined from deconvolution of XP C 1s
spectra, and the results are shown in Table 3. It can be
seen that the percentage of O–C=O determined from XPS
is similar to that of CO 2 -desorbing complexes shown in
Table 2. Both the percentages of C–O and O–C=O
decrease with the oxidation level, and the increase in
oxygen content upon oxidation is mainly contributed by
the formation of C=O, which would evolve as CO upon
thermal treatment. The XPS and TPD results of carbon–
oxygen complex analysis are qualitatively consistent with
each other.
3.2. Electrochemical performance of the resulting
capacitors
The cyclic voltammetric tests on the two-electrode
capacitors were conducted within a potential range of 20.6
to 0.6 V at different potential sweep rates. Figs. 1 and 2
shows the typical voltammograms of the capacitors fabri-
cated with different carbon fabrics. The figures demon-
strate that the electrodes are stable in the acid solution
within the potential range employed. Faradaic current
exhibiting as abrupt current increase was not observed in
the voltammogram for the CF capacitor. The intensity of
Faradaic current was found to increase with the increasing
oxygen extent of the electrodes, as inferred from the
gradual increase of anodic and cathodic currents at ca. 0.2
and 20.2 V, respectively, with the increasing extent of
oxygen treatment. The voltammograms also exhibit that
the induced current is an increasing function of the
oxidation level, indicating the increase of capacitance upon
oxidation.
Rectangular voltammograms, in which current quickly
reaches a truly horizontal value after reversal of the
potential sweep, were observed for the capacitor made of
CF. However, the delay for the current to reach a horizon-
670 C.-T. Hsieh, H. Teng / Carbon 40 (2002) 667 – 674
Fig. 1. Cyclic voltammograms of (a) CF and (b) CFO1 electrode
(2 cm 2 ) in 1 M H 2 SO 4 at different potential sweep rates.
Fig. 2. Cyclic voltammograms of (a) CFO2 and (b) CFO3
electrode (2 cm 2 ) in 1 M H 2 SO 4 at different potential sweep rates.
tal value near the reversal of the potential sweep and the
increase of slope in the horizontal region were enhanced
with the extent of oxidation. It is very likely that the
presence of surface oxides may retard the motion of
electrolytes and thus increase the ohmic resistance of
electrolytes along the axial direction of micropores, which
would combine with the existence of the distributed
capacitance to cause the delay of current inversion [21–
23]. The retarded electrolytic motion due to oxidation can
be partially supported by the observation that the acces-
sibility of the micropores to N 2 was hindered by the
introduction of the oxides, which results in the decreased
N 2 surface area and pore volume. In addition, surface
oxides are strong polar sites that would adsorb water
molecules and thus hinder the migration of electrolytes in
pores. Apart from the distributed capacitance effects,
Faradaic current may also hinder current inversion [22].
Since the voltammograms of the oxidized electrodes show
the presence of Faradaic currents, the surface oxides
created from the oxygen treatment may be responsible for
inducing chemical interactions (such as redox reactions)
between the carbon fabric and the electrolyte [1], which
will be discussed later in this paper.
Figs. 1 and 2 also show that both the anodic and
cathodic charging currents, Ia and Ic , respectively, are
increasing functions of the potential sweep rate in the
cyclic voltammetric measurements. The current plateaus of
Ia and Ic are parallel and the difference, DI (5Ia 2Ic ), was
found to be relatively invariant over the majority of the
potential range employed. The values of DI of different
capacitors obtained with different sweep rates are shown in
Fig. 3. DI is seen to be an increasing function of the
oxidation level, indicating an increase of capacitance upon
oxidation. The double-layer capacitance, Cdl , of the elec-
trodes can be estimated from the slope of the linear
relationship in Fig. 3 [24]. The calculated data are listed in
Table 4, showing that the capacitance increases slightly
with the oxidation level. The intercept of the linear plots of
DI against potential sweep rate represents the Faradaic
current [24], IF . The values of IF of these electrodes are
also compared in Table 4. It can be seen that IF was
significantly promoted through the introduction of oxygen
functional groups (from ca. 0 mA g 21 for CF to ca. 20 mA
g 21 for CFO3). Both Cdl and IF contribute to the total
capacitance. Faradaic current, the contributor of pseudo-
capacitance, may derive from some carbon–electrolyte
interactions, such as electrosorption and redox reactions
that are essentially reversible upon potential change [25].
Data in Table 4 show that the increase in double-layer
capacitance (Cdl ) due to oxidation is not obvious, while the
chemical interactions at the solid–liquid interface were
significantly enhanced with oxidation. It has been claimed
that the presence of Faradaic current would make it
difficult for the current to reach a truly horizontal value in
cyclic voltammetric tests [22]. This is in agreement with
the observation that deviation from rectangular shape of
 C.-T. Hsieh, H. Teng / Carbon 40 (2002) 667 – 674 671

Fig. 4. Comparison of charge–discharge curves of CF and CFO3

Fig. 3. Variation of DI (difference between anodic and cathodic electrodes (2 cm 2 ) at 0.5 m.
charging currents) with potential sweep rate in cyclic voltammetric
measurements using CF (n), CFO1 (1), CFO2 (,) and CFO3
(h) electrodes (2 cm 2 ). equivalent single-electrode capacitors in series. The
capacitances of different electrodes obtained with different
voltammograms was enhanced with the extent of carbon discharge currents are shown in Fig. 5. The capacitance
oxidation that has been found to induce the Faradaic decreases with discharge current, suggesting that the
current. potential difference between the mouth and the bottom of
To illustrate the influence of oxidation on the per- the micropores increases with the current due to ohmic
formance of constant-current charge and discharge, Fig. 4 resistance of the electrolyte in the axial direction of
shows the potential against time curves of the CF and micropores. As for the effect of oxidation, the specific
CFO3 capacitors charged and discharged at a constant capacitance was found to increase with the extent of
current of 0.5 mA. The CFO3 capacitor has a higher
capacitance for both charge and discharge, but possesses a
larger ‘IR drop’ at the beginning of discharge. Based on
the results of charge–discharge cycling, the specific dis-
charge capacitance of a single electrode in the capacitors
can be calculated according to:

C 5 (2It) /(WDE)

where I is the discharge current, t the discharge time, W

the carbon fabric mass on an electrode and DE the
potential difference in discharge, excluding the portion of
IR drop. The factor of 2 comes from the fact that the total
capacitance measured from the test cells is the sum of two

Table 4
Double-layer capacitance and Faradaic current of the carbon
electrodes determined from cyclic voltammograms
Carbon type Cdl (F g 21 ) IF (mA g 21 )
CF 121 0.082
CFO1 123 5.7
Fig. 5. Variation of specific discharge capacitance with discharge
CFO2 123 7.5
current for different electrodes (2 cm 2 ) charged at 0.5 mA to 0.6
CFO3 130 22
V.
672 C.-T. Hsieh, H. Teng / Carbon 40 (2002) 667 – 674

oxidation, which is in agreement with the results from
cyclic voltammetric measurements. A previous study has
also reported an increase of capacitance resulting from
electrochemical oxidation of carbon electrodes [26]. Com-
paring the capacitances of CF and CFO3 shows that there
is ca. 25% capacitance increase achieved through intro-
duction of surface oxides (e.g., an increase from 120 to
150 F g 21 at a current of 1 mA, or a current density of 0.5
mA cm 22 ).
In an ideal formation of electric double layer with acids
serving as the electrolyte, the equilibrium reaction at the
negative electrode during charging is simply presented as:
. Cx 1 H 1 5 . Cx / / H 1
where .C x represents the carbon electrode surface, H 1
the proton of the acidic electrolyte, and .C x / / H 1 the
double layer where the charges are accumulated on the two
sides of the double layer. The process is due to a simple
physical adsorption, by electrostatic forces between the
carbon surface and the proton. Basically, the numbers of
ions involved in building the double layer match the
charge density developed on the electrodes.
The data of the present work suggest that, as the extent
of oxidation increases, surface oxides would provide more
available sites for proton adsorption in the micropores of
the carbon fabrics. The preceding analysis of oxygen
functional groups has shown that oxidized carbons contain
a significant amount of carbonyl- or quinone-type groups,
i.e., C=O, on the surface. With the presence of these
groups, an equilibrium reaction may occur in carbon
electrode [1]:
. Cx O 1 H 1 5 . Cx O / / H 1
polarity, i.e., a surface electrostatic field, to carbons
[1,25,27,28]. The interaction of the electrostatic field at the
surface with the dipole moment of water molecules plays
an important role in determining the wettability of carbons
in aqueous solutions. It is generally recognized that the
micropores of carbons cannot be fully wetted in aqueous
solutions, and thus are not fully accessible to electrolyte or
hydrated molecules in the liquid phase. The increase in
oxygen content of the carbon fabric may improve the
wettability of the internal structure of micropores in the
carbon electrodes, thus resulting in a corresponding in-
crease in specific capacitance.
A sudden potential drop at the very beginning of the
constant current discharge is usually observed for EDLCs,
and this drop has been designated as the IR drop. This
potential drop has been attributed to the resistance of
electrolytes and the inner resistance of ion migration in
carbon micropores [29]. The latter usually has a higher
contribution to the whole IR drop. Assuming that the inner
resistance is one of the intrinsic characteristics of the
carbon electrodes, the potential drop measured should be
proportional to the discharge current. Fig. 6 shows the
variation of the IR drop with the discharge current for the
different electrodes. It can be seen that the potential drop
increases linearly with the current, and the slope of this
linear relationship was used to estimate the inner resistance
of the electrodes. The resistance is an increasing function
of the oxidation level, with resistances of 22, 30, 35 and 57
V for CF, CFO1, CFO2 and CFO3, respectively, in
agreement with the results using electrochemical oxidation
[26]. This result suggests that the imparted polarity may
hinder the motion of ionic species. The increase in the
resistance does not play a role in affecting the specific

where .C x O / / H 1 represents a proton adsorbed by a

carbonyl or quinone-type site, basically induced by ion-
dipole attraction. This specific adsorption process, which is
different from the formation of .C x / / H 1 on non-specific
sites through dispersion interactions [12,15], may facilitate
an excess specific double layer capacitance due to the local
changes of electronic charge density. It is thus suggested
that the increase of capacitance upon oxidation arises
partially from the enhanced dipole affinity towards protons
in an acid solution.
In charging the negative electrode, a strong bond may
also form between quinone-type groups and protons due to
electron transfer across the double layer:
. C x O 1 H 1 1 e 2 5 . C x OH

where .C x OH represents a hydroquinone-type complex

and e 2 an electron. The reaction would proceed backwards
during discharge. This type of functional groups, which
would provide redox activity, may be responsible for IF
and thus the pseudocapacitance component of the overall
capacitance of these oxidized carbon electrodes [25]. Fig. 6. Variation of IR drop with discharge current for electrodes
In addition, oxygen functional groups impart a surface (2 cm 2 ) charged at 0.5 mA to 0.6 V.
 C.-T. Hsieh, H. Teng / Carbon 40 (2002) 667 – 674
capacitance during the constant-current charge–discharge
cycling, since the IR drop has been excluded in capaci-
tance calculation. However, increasing the resistance
would result in a higher potential drop and thus a reduction
of specific capacity (in units of mA h g 21 ) of the
electrodes, especially at a high current density.
The leakage currents of CF and CFO3 capacitors
charged at 1 mA were measured at 0.6 V floating as shown
in Fig. 7. The current decreased gradually with time from 1
mA to around 1310 22 mA in 12 h. Sample CFO3 has a
higher leakage current than CF throughout the entire
period of measurement. The steady-state currents deter-
mined after 12 h of charge were 1.1310 22 and 9.4310 23
mA for CF and CFO3, respectively. The steady-state
current may be ascribed mainly to electronic current that
results from irreversible decomposition of electrolyte
components. It should be noted that this electronic current
is not included in IF that derives from the reversible
interactions between carbon and electrolyte. The increase
of leakage current suggests that the oxygen functional
groups may serve as active sites that catalyze the the
electrochemical oxidation or reduction of carbon or the
decomposition of electrolyte components [1,30].
The stability of the prepared capacitors can be examined
by conducting repeated charge–discharge cycling. A
capacitor equipped with CFO3 electrodes was charged and
discharged between 0 and 0.6 V at 1 mA to confirm the
stability. The coulombic efficiency (h ) of an electric
double-layer capacitor can be calculated from the equation
[31]:
h 5 (t D /t C ) 3 100
Fig. 7. Variation of leakage current with time for CF and CFO3
electrodes at a floating potential of 0.6 V.
673
Fig. 8. Variation of capacitance stability and coulombic efficiency
with cycle number for CFO3 electrode (2 cm 2 ) charged and
discharged at 1 mA in 1 M H 2 SO 4 .
where t D and t C are the times required for discharge and
charge, respectively. The variations of discharge capaci-
tance and coulombic efficiency with cycle number are
shown in Fig. 8. The results exhibit that the capacitor has
stable capacitance (about 150 F g 21 ) and coulombic
efficiency (about 99.5%) over 100 cycles.
4. Conclusions
The present work has demonstrated that the capacitance
of PAN-based carbon fabric in H 2 SO 4 can be enhanced
with oxygen treatment at 2508C. The results of N 2
adsorption showed that the oxygen treatment has little
influence on the physical characteristics of the carbon.
Surface analysis using TPD and XPS showed that the
amount of surface oxides increased with the extent of
oxygen treatment and the increase was contributed mainly
by the formation of carbonyl- or quinone-type groups that
normally desorb as CO during TPD. Cyclic voltammetric
study on the resulting electrodes showed that the Faradaic
current, the contributor of pseudocapacitance, increased
significantly with the extent of oxygen treatment, while the
increase in the double-layer capacitance was minor. Con-
stant current charge–discharge cycling reflected the impor-
tance of the distributed capacitance effects of these porous
electrodes, which was inferred from the decrease in
capacitance with the discharge current. Due to the treat-
ment with oxygen, the overall specific discharge capaci-
tance was found to have an increase up to 25% (e.g., from
120 to 150 F g 21 at a current density of 0.5 mA cm 22 ),
while both the resistance determined from the IR drop and
the leakage current increased with the extent of oxidation.
It is suggested that increasing the population of carbonyl-
674 C.-T. Hsieh, H. Teng / Carbon 40 (2002) 667 – 674
or quinone-type surface groups through oxygen treatment
is beneficial for capacitance promotion, but the advantage
can be offset with the coupling increases in inner resist-
ance and leakage current. The capacitors prepared in the
present work exhibit excellent capacitance stability with a
coulombic efficiency of 99.5% over 100 cycles.
Acknowledgements
Financial support from the National Science Council of
Taiwan is gratefully acknowledged. The project number is
NSC 89-2214-E-006-041.
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