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de
Porous 3D Few-Layer Graphene-like Carbon for
Ultrahigh-Power Supercapacitors with Well-Defined
Structure–Performance Relationship
Jin Zhao, Yufei Jiang, Hao Fan, Meng Liu, Ou Zhuo, Xizhang Wang,* Qiang Wu,*
Lijun Yang, Yanwen Ma, and Zheng Hu*
Electrical double layer capacitors (EDLCs), also called superca-
pacitors, have attracted much attention due to their capability
of delivering high power density and long cycling stability as
compared to batteries.[1] In principle, an ideal EDLC electrode
material should simultaneously meet the requirements of:
(i) a high specific surface area (SSA) to ensure the space for
charge storage, (ii) well-balanced pore distribution to improve
both specific capacitance and rate capability, (iii) high conduc-
tivity to ensure high rate capability and power density, and
(iv) good wettability to facilitate ion diffusion and increase the
ion-accessible surface area.[1,2] sp2 carbon materials are the
most commonly used electrodes due to their good conductivi-
ties, abundant structures and morphologies, easily modified
electronic structures and surface properties by doping and/or
surface functionalization.[2,3] Among reported sp2 carbon, gra-
phene has been widely studied as an attractive electrode mate-
rial owing to its high conductivity, high theoretical values of
SSA, and specific capacitance.[4] However, the inevitable π–π
aggregation and restacking of graphene sheets greatly limits
the electrolyte transfer and ion-accessible surface area, which
severely deteriorates the performance. Fabricating stable 3D
graphene to avoid this kind of restacking is an effective method
to excavate the supercapacitive potential of graphene.[4]
By an in situ MgO template method, we recently reported
novel 3D hierarchical carbon-based nanocages with featured
large SSA, coexisting micro-meso-macropores, and good con-
ductivity.[5] The pure carbon nanocages demonstrate high super-
capacitive performance.[5a] By doping nitrogen to introduce CN
polar bonds and improve wettability of the nanocages, the per-
formance is further enhanced to a top level.[5b] We noticed that
improving the wettability by N-doping is at the expense of con-
ductivity to some extent.[5b] Thus, if the high conductivity can be
Dr. J. Zhao, Dr. Y. Jiang, H. Fan, M. Liu, O. Zhuo,
Prof. X. Wang, Prof. Q. Wu, Prof. L. Yang, Prof. Z. Hu
Key Laboratory of Mesoscopic Chemistry of MOE
and Jiangsu Provincial Lab for Nanotechnology
School of Chemistry and Chemical Engineering
Nanjing University
Nanjing 210023, China
E-mail: wangxzh@nju.edu.cn; wqchem@nju.edu.cn;
zhenghu@nju.edu.cn
Prof. Y. Ma
Jiangsu Key Lab for Organic Electronics and Information
Displays & Institute of Advanced Materials
Nanjing University of Posts and Telecommunications
Nanjing 210046, China
DOI: 10.1002/adma.201604569
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maintained or even enhanced with increasing wettability, there
will be a big space for further improvement of supercapacitive
performance. As known, graphene grown on a metallic tem-
plate usually has higher crystallinity and better conductivity than
that grown on an oxide template.[6,7] Based on these considera-
tions, herein we have developed an in situ porous Cu template
method to prepare 3D hierarchical porous carbon nanomaterials
in analogy to the in situ MgO template method. The unique 3D
few-layer graphene-like carbon (3DG) is obtained which is char-
acterized by the open porous architecture with interconnected
micro-meso-macropores, large SSA (>1500 m2 g−1), high con-
ductivity (>800 S m−1), and high wettability either in aqueous
or in ionic liquid electrolytes. As a result, 3DG presents the high
supercapacitive performances in both the electrolytes. Especially,
EDLCs based on the 3DG prepared at 1000 °C deliver ultrahigh
maximum power densities of 1066.2 and 740.8 kW kg−1 in
aqueous and ionic liquid electrolytes, respectively, with a top-
level energy density, rate capability, and cycling stability. The
excellent performance is well-associated with the unique struc-
ture by detailed examination on the changing behavior of equiv-
alent series resistance (RESR) with current density combined
with the classical electrochemical impedance spectroscopy.
The 3DG prepared at 800, 900, and 1000 °C are denoted as
3DG800, 3DG900, and 3DG1000, respectively. Figure 1 shows
the typical morphological and structural characterizations of
3DG1000. Basically, 3DG1000 maintains the profile of the 3D
porous Cu template inherited from the basic copper carbonate
precursor, and demonstrates a core–shell structure with abun-
dant open pores of different sizes in either the shell or the core.
The porous morphology for meso- and macropores exhibits a
self-similarity of irregular fractal as shown in the scanning elec-
tron microscopy (SEM) images with different magnifications,[8]
and the shell is denser than the core (Figure 1a–f and Figure S1
(Supporting Information)). Transmission electron microscopy
(TEM) observations further reveal that the hierarchical pores
are composed of the interconnected crumpled sheets of one
to three graphitized layers in thickness (Figure 1g,h). 3DG800
and 3DG900 exhibit similar features (Figure S2, Supporting
Information). The steep uptake at p/p0 < 0.01 in the N2 sorp-
tion isotherm indicates the existence of abundant micropores.
The crescent-like hysteresis loop at 0.42 < p/p0 < 1 exhibits no
limiting adsorption at high p/p0 and no clear boundary between
the sorption regions corresponding to meso- and macropores
(Figure 1i and Figure S3 (Supporting Information)). This is
a typical type H3 loop, confirming a loose network and coex-
isting micro-meso-macropores for the 3DG.[9] This isotherm is
somewhat different from that of the carbon-based nanocages
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Figure 1.  Morphological and structural characterizations of 3DG1000. a–f) SEM images with different magnifications for the shell (a–c) and the core
(d–f). g,h) TEM images. Inset in (h) is the corresponding high-resolution TEM image. i) Nitrogen sorption isotherm. Inset is the corresponding pore
size distribution.

prepared by the in situ MgO template method where there
exists an obvious bottleneck between the sorption regions
corresponding to meso- and macropores (Figure S4, Sup-
porting Information).[5] These results indicate that the in situ
Cu template method provides a new 3DG characterized by an
open porous architecture with interconnected micro-meso-
macropores. Such a unique framework avoids the π–π aggre-
gation and restacking of graphene sheets, and favors the high
SSA, high pore volume, and high conductivity, hence it could
provide sufficient space for charge storage and fast channels for
charge (ions and electrons) transfer. Actually, the interconnec-
tivity of the open micro-meso-macropores is particularly attrac-
tive for the convenient ion diffusion and adsorption which is
crucial for supercapacitive performance.[4b,10] With increasing
growth temperature, the SSA increases from 1325 to 1450 and
1545 m2 g−1, and the total pore volume increases from 5.04 to
6.62 and 7.30 cm3 g−1 for 3DG800, 3DG900, and 3DG1000,
respectively (Table S1, Supporting Information). Such temper-
ature dependences may be attributed to the stronger etching
effects of hydrogen on carbon[11] and the larger template size
at higher temperature, correspondingly. As expected, the
conductivity associated with the crystallinity also increases
with increasing growth temperature, and reaches 828 S m−1
for 3DG1000 which is obviously higher than the typical range
of 60–500 S m−1 for the graphene electrodes derived from gra-
phene oxide (Figure S5, Supporting Information).[4a,12]
In addition to the unique geometric characteristics and high
conductivity, the wettability of the 3DG is also quite attractive.
Figure 2 presents the dynamic contact angle measurements for
either water or ionic liquid droplets of 1-ethyl-3-methylimida-
zolium tetrafluoroborate (EMIMBF4) on 3DG1000. For com-
parison, the corresponding measurements on the annealed
3DG1000 in Ar at 1000 °C for 1 h (designated as a-3DG1000)
were also presented (Figure S6, Supporting Information). As
known, the pure carbon materials are usually very hydrophobic,
e.g., the pure carbon nanocages present an almost unchanged
contact angle of ≈126°.[5b,13] Interestingly, 3DG1000 is quite
hydrophilic with an initial contact angle of 94.6° and the droplet
is completely absorbed within 90 s (Figure 2a). This results
from the introduced polar oxygen-containing groups during
the removal of the Cu template as revealed by X-ray photo-
electron spectroscopy characterization (Figure S7, Supporting
Information).[13c,14] By annealing 3DG1000 to remove the
groups, the a-3DG1000 sample recovers the very hydrophobic

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Figure 2.  Dynamic contact angle measurements for 3DG1000 and a-3DG1000: a) for water, b) for EMIMBF4.
feature with an almost unchanged contact angle of 134.5°. The
wettability of 3DG1000 for EMIMBF4 is even better, as reflected
by the small initial contact angle of 51.3° and fast complete wet-
ting within ≈30 s. Different from the case in water, a-3DG1000
still keeps the very good wettability in EMIMBF4, only slightly
inferior to that of 3DG1000 (Figure 2b).
The preceding results indicate that the in situ Cu template
method provides a unique architecture of porous 3DG with
high conductivity and wettability, which satisfies the gen-
eral requirements for ideal EDLC electrode materials. Thus,
the supercapacitive performances of 3DG800, 3DG900, and
3DG1000 were evaluated by two-electrode coin-type superca-
pacitors either in potassium hydroxide (KOH) aqueous elec-
trolyte or in EMIMBF4. The corresponding supercapacitors are
denoted as 3DG800-SC, 3DG900-SC, and 3DG1000-SC.
As shown in Figure 3, in a KOH aqueous electrolyte, 3DG1000-SC
presents excellent rectangle-like cyclic voltammetry (CV) curves
without a very oblique angle even at a scan rate as high as
10 V s−1, indicating ideal capacitive behavior with a high rate capa-
bility and a small RESR (Figure 3a).[5a,b] In general, 3DG900-SC
and 3DG800-SC also exhibit rather good capacitive behavior, but
slightly inferior to 3DG1000-SC. At the scan rate of 0.1 V s−1,
the specific capacitance decreases from 219 F g−1 for 3DG1000
to 196 F g−1 for 3DG900 and 175 F g−1 for 3DG800 (Figure 3b
and Figure S8 (Supporting Information)). Galvanostatic charge/
discharge (GCD) curves show highly symmetry and nearly
linear slopes even at the high current density of 100 A g−1 with
rather limited voltage (IR) drops of 0.116, 0.047, and 0.028 V
for 3DG800-SC, 3DG900-SC, and 3DG1000-SC, respectively,
which also indicates the ideal capacitive behavior (Figure 3c and
Figure S9 (Supporting Information)). The corresponding curves
of specific capacitance versus charge/discharge current density
indicate their high rate capabilities with 3DG1000-SC the best
(Figure 3d), in agreement with the CV characterization results
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(Figure 3a,b). At 1 A g−1, the specific capacitance of 3DG1000
reaches 231 F g−1, larger than 213 F g−1 of 3DG900 and 189 F g−1
of 3DG800, which locates at the top level for carbon-based mate-
rials (Figure S10, Supporting Information).[3,4,15] Even increasing
the current density to an ultrahigh value of 2000 A g−1, 3DG1000
still maintains a high specific capacitance of 129 F g−1, ≈56%
of its initial capacitance, at the state-of-the-art level to date
(Figure 3d and Figure S9f (Supporting Information)).[12c,16] In
addition, 3DG1000-SC displays an excellent stability of ≈99%
capacitance retention after 20 000 cycles at the high current den-
sity of 100 A g−1 with Coulombic efficiency of ≈100% (Figure 3e).
Such a high cycling stability is correlated with its hierarchical
open porous architecture which could avoid the π–π aggrega-
tion and restacking of graphene sheets and accommodate the
deformation of the framework.[5d,8b,17] Also, Ragone plots fur-
ther demonstrate the best performance of 3DG1000-SC which
delivers an energy density of 4.2 Wh kg−1 at an ultrahigh average
power density of 123.1 kW kg−1 (Figure 3f).
To understand the origin of the advanced supercapacitive
performance, we used two approaches to determine the struc-
ture–performance relationship of the supercapacitors as shown
in Figure 4. Based on the GCD curves at different current den-
sities, RESR from IR drop and corresponding maximum-power
density (Pmax) were obtained (Figure 4a,b). It is worth noting
that, with increasing current density, RESR first decreases gradu-
ally to a minimum and then rebounds with a slight tendency
to a relatively stable value for all the three supercapacitors
(Figure 4a). Such a changing behavior of RESR has never been
reported before to our knowledge, which should be associated
with the unique structure of the 3DG in this study. As known,
RESR is mainly composed of three parts, i.e., the intrinsic
Ohmic resistance (Rs), the interfacial charge transfer resistance
(Rct), and the Warburg diffusion resistance (Rw). Rs is little
changed with the current density. On the contrary, Rct and Rw
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b c
300 300
Specific Capacitance (F g )

1.0

Specific capacitance (F g )
-1

-1

-1
1Ag
3DG1000 3DG1000
200 250 3DG900 0.5
-1 3DG900
0.1 V s 3DG800 3DG800
100 200

Voltage (V)
-1
1Vs 0.0
2Vs
-1 0 50 100 150 200 250
0 -1
150 1.0 -1
5Vs 100 A g
-1
-100 10 V s 100
0.5
-200 50
-300 0 0.0
0.0 0.2 0.4 0.6 0.8 1.0 0 5 10 15 20 0.0 0.5 1.0 1.5 2.0 2.5
Voltage (V)
-1
Scan rate (V s ) Time (s)

d e f 6
300 120 10
Specific Capacitance (F g )
-1

Power Density (W kg )
3DG1000 Coulombic efficiency

-1
250 3DG900 Capacitance retention 10
5
Percentage (%)

3DG800 100
200 4
10
150
80 10
3
3DG1000
100 3DG900
2
50 10 3DG800
60
1
0 10
0 500 1000 1500 2000 0 5000 10000 15000 20000 0 1 2 3 4 5 6 7 8
-1 -1
Current Density (A g ) Cycle Number Energy Density (Wh kg )

Figure 3.  Supercapacitor performances of 3DG800, 3DG900, and 3DG1000 in 6 mol L−1 KOH. a) CV curves of 3DG1000-SC at different scan rates.
b) Specific capacitance versus scan rate. c) GCD curves at the current densities of 1 and 100 A g−1. d) Specific capacitance versus current density.
e) Cycling stability and Coulombic efficiency of 3DG1000-SC at 100 A g−1. f) Ragone plots of the average-power density versus energy density of
supercapacitors.

a b
1.0 3DG1000
3DG900 6
10
Pmax (W kg )

0.8 3DG800
-1
RESR (Ω)

0.6
5
10
0.4 3DG1000
3DG900
0.2 3DG800
4
0.0 10
1 10 100 1000 1 10 100 1000
-1
-1
Current Density (A g ) Current Density (A g )

c 10 d -100
3DG1000 3DG1000
Phase angle (degree)

3DG900 3DG900
3DG800 -80
3DG800
3
-Z'' (Ω)

-60
5 2
-40 τ0=236 ms
1
τ0=124 ms
-20
0 τ0=60 ms
0.0 0.5 1.0
0 0 -2
0 5 10 -1 0 1 2 3
10 10 10 10 10 10
Z' (Ω) Frequence (Hz)
Figure 4.  Two approaches to the structure–performance relationship of the supercapacitors in 6 mol L−1 KOH. a,b) RESR from IR drop and the respec-
tive maximum-power density versus current density. c,d) Nyquist plots and the respective Bode plots. Inset in (c) magnifies the high-frequency range.

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are associated with the ion diffusion either in the electrolyte
or at the electrolyte–electrode interface, thus are sensitive to
the morphology and surface property of the electrode as well
as the current density related to the ion migration (Figure S11,
Supporting Information).[1a,18] At a low current density, the
micropores will fully contribute to charge storage but within
which the ion diffusion and transfer is difficult, leading to the
large Rct and Rw, thus the large RESR.[19] The smaller the cur-
rent density, the larger the Rct and Rw, and vice versa. Hence,
RESR increases with decreasing current density at the low cur-
rent density side (Figure 4a). When increasing the current den-
sity to a certain extent, the micropores will be partially blocked,
while the meso- and macropores are still accessible to ions
within which the ion diffusion and transfer is smooth and only
gets slightly difficult with increasing current density.[19] This
picture results in stable RESR with a slight increasing tendency
at the high current density side (Figure 4a). As learnt from
our characterizations, the higher growth temperature leads to
the higher conductivity favorable for the smaller Rs, and the
higher proportion of larger-sized pores (thus the larger meso-
and macropore volume) favorable for the smaller Rct and Rw
(Figures S5 and S3b and Table S1, Supporting Information).
As a result, the RESR value is in the order of 3DG1000-SC
< 3DG900-SC < 3DG800-SC, while the stability of RESR at high
current density side slightly increases with increasing growth
temperature (Figure 4a). Therefore, the changing tendency
of RESR versus current density reflects the unique morpho-
logical and structural features of the porous 3DG. For each
supercapacitor, the highest value of the maximum-power
density, Pmax, corresponds to the minimum RESR. Pmax reaches
1066.2 kW kg−1 at 20 A g−1 for 3DG1000-SC, which is a state-of-
the-art value for carbon-based supercapacitors (Figure 4a,b and
Table S2 (Supporting Information)).
The understanding from the last approach is supported by
classical electrochemical impedance spectroscopy. The nearly
vertical Nyquist plots in the low-frequency region demon-
strate the ideal capacitive behavior for all three supercapacitors
(Figure 4c).[5b] The enlarged high-frequency region presents a
transition from the vertical curve to the 45° Warburg region fol-
lowed by a semicircle (inset in Figure 4c). By extrapolating the
vertical portion to the real axis, the remarkably small RESR of 0.17,
0.33, and 0.67 Ω was obtained for 3DG1000-SC, 3DG900-SC,
and 3DG800-SC, respectively, in agreement with the highly rec-
tangle-like CV curves and very limited IR drops in GCD curves
(Figure 3a,c). Such small RESR values closely correlated with the
high conductivity, good wettability, and particularly the hier-
archical open porous architecture, which provides a rapid ion
diffusion channel and a short diffusion distance by the inter-
connected micro-meso-macropores.[10,18c,19] Actually, the RESR
values are even smaller than those of the ultrahigh-performance
supercapacitors based on the 3D hierarchical carbon-based
nanocages where the inside mesopores and outside macropores
are connected by the micropores across the graphitized shells
of the nanocages (Figure S4, Supporting Information).[5b] It is
noted that these RESR values are consistent with the respective
stable ones of ≈0.15, 0.24, and 0.60 Ω at the high current den-
sity side in Figure 4a, with the same relative order. This is due
to the fact that the RESR deduced from Nyquist plot corresponds
to a relatively high frequency and only the relatively large-sized
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pores can be accessed by ions, hence similar to the situation
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at high current density.[20] In the Bode plots, the character-
istic frequency f0 at the phase angle of −45° for 3DG1000-SC,
3DG900-SC, and 3DG800-SC is 16.6, 8.06, and 4.24 Hz, cor-
responding to the time constant τ0 (τ0 = 1/f0) of 60, 124, and
236 ms, respectively (Figure 4d). These τ0 values are greatly
smaller than those of the conventional activated-carbon super-
capacitors (≈10 s), indicating the faster charge/discharge rate of
the 3DG-based supercapacitors.[12c,16e,f ]
The best supercapacitive performance for 3DG1000 among
the three products is attributed to its larger SSA, larger pore
volume, and higher conductivity, which result in the largest
charge storage space and fastest charge (ion and electron)
transfer. In addition, the excellent wettability of 3DG1000 also
plays an important role, as evidenced by its much better super-
capacitive performance than that of a-3DG1000 (the annealed
sample) (Figure S12, Supporting Information). Especially, the
synergism of the open porous architecture of the intercon-
nected micro-meso-macropores, high conductivity, and good
wettability ensures the high rate capability of the products with
3DG1000 being the best.
As known, the energy stored in a supercapacitor is propor-
tional to the square of its operating voltage. Hence, we further
test the electrochemical performance of 3DG1000-SC in the
ionic liquid electrolyte of EMIMBF4 with a wide voltage window
of 0–4 V as shown in Figure 5. Both the rectangle-like CV curves
at high scan rates (0.5–2 V s−1) and the nearly symmetry GCD
curves with small IR drops at high current densities (0.94 V at
200 A g−1) indicate the ideal capacitive behavior and small RESR,
as confirmed by the nearly vertical curve in the low-frequency
region of Nyquist plot (Figure 5a–c). A high specific capacitance
of 226 F g−1 is obtained from the GCD curve at 1 A g−1, with
a area-normalized capacitance of 14.7 µF cm−2 (Figure S13,
Supporting Information). The very close specific capacitances
in the ionic liquid and the aqueous electrolytes are ascribed to
the better wettability of the unique 3DG in the former than in
the latter, which compensates the unfavorable influences of the
large ion size, low conductivity, and high viscosity of EMIMBF4
(Figure 2).[21] Increasing the current density up to 200 A g−1, the
specific capacitance still maintains 135 F g−1 with ≈60% reten-
tion, indicating the high rate capability as supported by the
small τ0 of 1.01 s (Figure 5c,d). The RESR obtained from Nyquist
plot is 2.56 Ω, in agreement with 2.35 Ω derived from the IR
drop at 200 A g−1, which is much smaller than those (6–15 Ω)
for the high-performance EDLCs with EMIMBF4 electrolyte
in literatures (Figure 5b,c).[22] This is also associated with the
unique structure of the 3DG. Due to the high specific capaci-
tance and wide operating voltage, 3DG1000-SC offers a high
energy density of 44.0 Wh kg−1 at a ultrahigh power density of
152.9 kW kg−1, much better than the case in aqueous electro-
lyte (Figures 3f and 5e). At 1 A g−1, the energy density reaches
125.5 Wh kg−1 with a power density of 1.0 kW kg−1. Assuming
a 30% weight ratio for active material in the packaged com-
mercial supercapacitor,[4a,23] the energy density of the device is
about 37.7 Wh kg−1, which is much larger than that for com-
mercial electrochemical capacitors (ECs). With the high energy
and power densities, the device could bridge the gap of ECs
and lithium ion batteries (Figure 5e).[3b,16f ] 3DG1000-SC with
EMIMBF4 electrolyte also exhibits a very good cycling stability
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b c
300 30
Specific Capacitance (F g )
-1

4 1Ag
-1

200 2Ag
-1
25
2 -100

Phase Angle (degree)

Voltage (V)
100 -1 20 -80
0.5 V s

-Z'' (Ω)
0 τ 0=1.01 s
0 1Vs
-1 0 200 400 600 800 1000 15
-60
-1 4 100 A g
-1 -40
2Vs
-100 200 A g
-1 10 -20
2 0
-200 5 -2 -1 0 1 2
10 10 10 10 10
Frequence (Hz)
-300 0 0
0 1 2 3 4 0 2 4 6 0 5 10 15 20 25 30
Voltage (V) Times (s) Z' (Ω)

d e
300 f
Specific Capacitance (F g )

6
10 120
-1

Capacitors
Power density (W kg )
Coulombic efficiency
-1

5 3DG1000-SC
250 10 Capacitance retention

Percentage (%)
4 100
200 10
3
10
150 Li-ion
80
2
10
Commercial ECs
100 10
1
60
0
50 10
0 50 100 150 200 0.01 0.1 1 10 100 0 5000 10000 15000 20000
-1 -1
Current Density (A g ) Energy density (Wh kg ) Cycle Number

Figure 5.  Supercapacitor performance of 3DG1000 in EMIMBF4. a) CV curves. b) GCD curves. c) Nyquist plot. Inset is the corresponding Bode plot of
phase angle versus frequency. d) Specific capacitances at different current densities. e) Ragone plots for 3DG1000-SC in comparison with traditional
capacitors, commercial ECs, and lithium-ion batteries.[3b,16f ] The data are based on all device mass (assuming a 30% weight ratio for active material).
f) Cycling stability and Coulombic efficiency at 100 A g−1.

of ≈91% capacitance retention after 20 000 cycles at a high cur- in situ porous Cu template method in this study, thus leading
rent density of 100 A g−1 with Coulombic efficiency of ≈100% to excellent supercapacitive performance.
(Figure 5f). The demonstration experiment shows a clear In summary, a unique 3D few-layer graphene-like carbon is
indicator over 6 h for a timer powered by 3DG1000-SC with prepared by a new in situ porous Cu template method, which
EMIMBF4 electrolyte (Figure S14, Supporting Information). integrates the features of open porous architecture with inter-
Different from the situation in aqueous electrolyte, the similar connected micro-meso-macropores, large specific surface area,
supercapacitive performances for 3DG1000 and a-3DG1000 are high conductivity, high stability, and good wettability either in
observed (Figures S12 and S15, Supporting Information). This aqueous or in ionic liquid electrolytes. The synergism of these
is ascribed to their similar pore structure, close SSA, and similar characteristics endows the sufficient space for charge storage
wettability in EMIMBF4 (Figure 2b and Figure S6 (Supporting and the ultrafast channels for charge transfer, thus the excellent
Information)). The maximum power density is estimated to be supercapacitive performance. The EDLCs based on 3DG1000
740.8 kW kg−1 according to the RESR obtained from the IR drop deliver the ultrahigh maximum power densities of 1066.2 and
at 20 A g−1, which is also at the top level for carbon-based super- 740.8 kW kg−1 in aqueous and ionic liquid electrolytes, respec-
capacitors (Table S2 and Figure S16, Supporting Information). tively, with top-level energy density, rate capability, and cycling
The preceding results demonstrate excellent supercapacitive stability. Especially, the state-of-the-art performances in ionic
performance of the porous 3DG with a top-level specific capaci- liquid electrolyte bridge the gap between traditional capacitors
tance and corresponding high energy density, state-of-the-art and batteries, indicating the great potential for applications.
power density, and high cycling stability in both aqueous and The correlation of the performance with structure is explored
ionic liquid electrolytes. Such an excellent performance results for the first time by examining the changing behavior of equiv-
from the large space for charge storage and the fast channels for alent series resistance with current density in detail, which
charge transfer, as well as the high structural stability due to the provides a deep insight into the structural features of the mate-
unique architecture of the porous 3DG. Actually, 3D graphene rials, thereof the performances. The knowledge obtained by
materials have attracted much attention in recent years due to this new angle is well supported by that obtained from classical
their wide potential applications,[12,24,25] but there still exists the electrochemical impedance spectroscopy. The combination of
big space from the viewpoint of supercapacitive energy storage. these two complementary approaches could extend and deepen
It was rather difficult to simultaneously meet the requirements the understanding on structure–performance relationships of
of large SSA, well-balanced pore distribution, high conductivity, the electrode materials not only for supercapacitors but also for
good wettability, as well as high stability.[12,24] Such a condition many electrochemical energy storage systems, e.g., Li-ion, Li–S,
is achieved with the unique porous 3DG prepared by the new metal–air batteries, which is of great significance.

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Supporting Information
Supporting Information is available from the Wiley Online Library or
from the author.
Acknowledgements
This work was jointly supported by the NSFC (51232003, 21373108,
51571110, 21473089, 21573107), the “973” Program (2013CB932902),
the Suzhou Program (ZXG2013025), the Changzhou Technology
Support Program (CE20130032), and the Priority Academic Program
Development of Jiangsu Higher Education Institutions.
Received: August 26, 2016
Revised: November 15, 2016
Published online:
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