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Ordered mesoporous carbon and its applications

Cite this: Mater. Chem. Front.,
2017, 1, 1001
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for electrochemical energy storage
and conversion
Ali Eftekhari*ab and Zhaoyang Fanc

Received 7th November 2016,
Accepted 4th January 2017
DOI: 10.1039/c6qm00298f
rsc.li/frontiers-materials
Ordered mesoporous carbon (OMC) is a flexible material providing interconnected channels for the diffusion of
electroactive species in electrochemical systems. This is a unique feature, which distinguishes OMC from other
types of carbonaceous materials including mesoporous carbon (MC). The potential of OMC in electrochemical
systems has been overshadowed by the vague terminology of this class of mesoporous materials. Despite the
ordered structure of mesopores, the electrochemistry of OMC is not straightforward. This manuscript reviews
the opportunities experimentally presented for employing OMC in various electrochemical power sources such
as ultracapacitors, supercapacitors, battery systems, fuel cells, and electrochemical hydrogen storage systems.
The aim is to highlight its potential and critical issues. For instance, the graphitization of OMC is of particular
importance, as the ordered alignment of p electrons can be beneficial for charge transfer, while the mesopore
edges can resemble the peculiar properties of graphene edges.

1. Introduction
Owing to its unique flexibility in forming nanostructures,
a
The Engineering Research Institute, Ulster University, Newtownabbey BT37 OQB, carbon has found a central role in the realm of nanotechnology,
UK. E-mail: eftekhari@elchem.org with fullerenes, carbon nanotubes, and graphene as the land-
b
School of Chemistry and Chemical Engineering, Queen’s University Belfast,
mark discoveries.1 A new member of this family is ordered
Stranmillis Road, Belfast BT9 5AG, UK
c
Department of Electrical & Computer Engineering and Nano Tech Center, Texas mesoporous carbon (OMC), which has recently attracted con-
Tech University, Lubbock, Texas 79409, USA. E-mail: zhaoyang.fan@ttu.edu siderable attention.

Ali Eftekhari is a professor of Dr Zhaoyang Fan obtained his

chemistry temporarily in the
University of Ulster and Queen’s
University Belfast. He has worked
in different capacities in various
universities across 4 continents
and founded two internationally
recognized academic schools from
scratch, which were considered as
exceptional success stories by
major media such as the British
newspaper, The Guardian. His
Ali Eftekhari research interest is focused on
material design for electro-
chemical systems and he has worked on energy storage systems
for 20 years. He is the principal author of over 100 papers
published in leading scholarly journals and has supervised over
110 postdoctoral researchers and graduate students. He is the
President of the American NanoSociety.
bachelor and master degrees from
the Tsinghua University of China
and PhD from the Northwestern
University of US. He is currently
an associate professor in the
Department of Electrical and
Computer Engineering and
NanoTech Center, Texas Tech
University. His current research
concerns synthesis and property
studies of nanomaterials and
Zhaoyang Fan semiconductor thin films, and
their application development for
photonic devices, photovoltaics,
and electrochemical energy storage
systems.

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Review
On the other hand, porous carbon materials, although not
so exciting, have a much longer practical application history.
With their remarkable physicochemical properties, including a
large specific surface area (SSA) and pore volume, high corrosion
resistance, and good thermal and mechanical stabilities, and
further considering their easy manufacturing and the abundance
of their precursors on Earth, porous carbon materials have been
employed in various applications. These include water and air
filtration, as catalysts or catalyst supports, as gas storage hosts, and
in electrochemical energy storage and conversion systems. They
are still dominant characteristic materials for such applications.
According to the IUPAC classification of porosity, micro-
pores are o2 nm, mesopores are in the range of 2–50 nm, and
macropores are 450 nm. Traditional porous carbon materials,
including activated carbons and carbon molecular sieves, are
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commonly synthesized using a pyrolysis process with appro-
priate carbon precursors such as coal, polymers, and carbides,
with activation through potassium hydroxide2 or selective
etching of metal ions in carbides by halogen gases.3 Associated
with these micropore-dominated carbon materials are draw-
backs that include slow mass transport in the micropores, low
electrical conductivity resulting from abundant surface groups
and defects, and porous structure collapse at high temperature,
among others.
From the consideration of molecule diffusion and electro-
lyte ion transportation, mesoporous carbon (MC), which is
dominated by 2–50 nm mesopores, is more interesting, since
micropores might not be easily accessible by these species,
while macropores are simply too large leading to a reduced SSA.
Therefore, MC was subsequently developed through a variety
of strategies.4–9 This MC material has a broad pore-size distribu-
tion without structural ordering (or symmetry). Indeed, MC is a
general category according to the physical porosity and does not
necessarily represent the same geometrical structure. The meso-
porosity of carbon in the form of nanostructured texture obviously
increases the specific surface area. Of course, the disordered pores
are unpredictable in electrochemical performance, as the pores
are not necessarily electrochemically accessible.
OMC certainly can be regarded as a natural evolution from
MC when constraints of narrow pore size distribution with
ordered pore positions are applied. Strictly speaking, if a perfect
ordering is defined for a specific pore size on a macro-scale, such
OMC will belong to the category of superlattices or meta-
materials with unique properties due to its 2D or 3D periodical
structure resulting in quantization of wave vectors (i.e. dramati-
cally different from MC with a random pore size and a random
pore position). However, from a practical point of view in
electrochemistry, neither a perfect pore ordering nor the same
pore size is necessary. OMC, with either a non-perfect ordering
or a non-uniform pore size, due to the easier fabrication and
control, is under active investigation for much better perfor-
mance in many applications that traditionally employ MC or
porous carbon. This is particularly true for electrochemical
energy conversion and storage. The explosive increase in the
number of papers published in the very recent few years illus-
trates the research interest in this field.
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In this review, we will first summarize the synthesis methods
and novel OMC properties, and then focus on its applications for
electrochemical energy conversion and storage, including super-
capacitors, lithium-ion batteries (LIBs), and other emerging
rechargeable batteries.
2. Ordered mesoporous carbon:
synthesis and properties
2.1. From mesoporous carbon to ordered mesoporous carbon
Mesoporous carbons could be synthesized by different methods,
such as catalytic activation of carbon precursors using metal-
containing species,9,10 carbonization of the blends of one thermo-
setting precursor and one thermally unstable polymer,7 and
carbonization of organic aerogels.11 The produced mesopores
from these methods generally have a broad size distribution.
They also introduce a lot of micropores. Well-controlled pore
size distribution through a template method, therefore, became
more interesting.
The story was started by attempts at utilizing silica gel as the
template for the preparation of carbonaceous materials. In the
1980s, synthesis of MC was investigated by impregnating a
phenol–hexamine mixture as a carbon precursor into silica gel
as a template.12 Owing to the spacious structure of silica gel,
the carbon precursor can be easily inserted. Upon the completion
of the carbonization process, the silica template can then be easily
removed. Although the resulting MC has no structural ordering
(symmetry), this effort provided the strategy of template-guided
OMC synthesis, as long as an ordered template with suitable
dimensions is available. Liquid crystals provide an ordered struc-
ture with the mobility of a liquid, which can be used as a
mesoporous template. This feature was utilized in 1992 to
fabricate mesoporous molecular sieves13,14 and led to the birth
of an interesting family of ordered mesoporous materials with
crystal-like symmetries. Carbon is usually a pioneer in forming
new nanostructures, but cannot be synthesized chemically in a
liquid through the liquid crystal template. Hence, OMC is synthe-
sized by utilizing the mesoporous silica templates originally
prepared using the liquid crystal template.15–17 For about two
decades starting in the 1980s,12,18,19 various silica and zeolite
templates were utilized for the preparation of MC. The birth of
OMC did not happen until 1999 when cubic mesoporous alumino-
silicate MCM-48 was employed as the hard template,15,20 thus
creating a new nanocarbon structure with symmetry. Currently,
OMC that has a very narrow pore-size distribution with periodical
structural ordering is synthesized using a template. Depending on
the template used, the OMC synthesis can be differentiated into
two categories: hard-templating based (impregnation and etching
back) and soft-templating based (direct synthesis). Their major
differences are illustrated in Fig. 1.
2.2. OMC synthesis: hard-template based
In this strategy, an ordered mesoporous solid template is applied
as the mold for the negative replication of OMCs. The pore size
control and symmetric ordering are simply determined using the

Materials Chemistry Frontiers
Fig. 1 Schematics comparing (a) hard-template based and (b) soft-
template based synthesis strategies. Reproduced with permission from
ref. 19. Copyright 2006, Wiley-VCH.
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solid template and do not rely on the interaction between the
carbon precursor and the template.
The development of hard-template based OMCs was com-
prehensively reviewed by Dai et al.4 In this hard-templating
synthesis strategy,19 a preformed hard template, particularly a
silica based ordered mesoporous structure, is used, and carbon
precursors are impregnated into the pore volume. After carbo-
nization, the hard template is etched away, leaving the
negatively replicated OMC. That is, the interconnected pore
space in the template is transferred into the continuous frame-
work of the OMC, while the volume once occupied by the
template material becomes mesopores in the OMCs. The 3D
interconnected porous structure of the template is generally
considered to be necessary for this process. The success of
using an SBA-15 silica mesoporous molecular sieve as a template,
which has a cylindrical pore structure, is due to the existence of
interconnecting micropores in the sidewalls. It is worth mention-
ing that, in addition to the solution-based impregnation to fill the
precursor into the pore volume of the template, chemical vapor
deposition was also capable of filling the pore volume.
Template candidates. Silica-based order mesoporous struc-
tures such as MCM, SBA, FDU, MSU-H, and HMS series have
contributed to the synthesis of a variety of OMC structures such
as cubic structures with several symmetries, face-centered
cubic, body-centered cubic, and 2D hexagonal structures. Some
efforts have also been focussed on the use of as-synthesized
ordered structures of colloid nanoparticles (NPs) as the hard
templates. The OMC pore size now is primarily determined by
the NP size, and therefore, the pore size can be easily adjusted
in a large range.21 Silica NPs, polymer beads such as polystyrene
spheres and others can be used. Iron oxide NPs are interesting22
since iron can catalytically induce graphitization at lower tem-
peratures (o1000 1C).23
The key advantage of silica-based templates is the highly
ordered architecture of the mesopores, but a key disadvantage
is the essential requirement of acid treatment for the template
removal. The strong acid treatment does affect the carbon
surface and its functionality. This is similar to the undesirable
acid treatment required for the removal of the catalyst and
catalyst support after chemical vapor deposition of carbon
nanomaterials.24 Although the defects formed might be useful
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in the electrochemical system, the material ordered architec-
ture is lost at the atomic scale. Other templates such as MgO
have also been introduced,25–27 which can be removed using a
light acid treatment, but the uniformity of the mesopores is not
at the level of silica-based templates. However, another con-
siderable advantage of such templates is a practical feasibility
for scaling up the material production.
Carbon precursors. During the high-temperature carboniza-
tion and graphitization process, the molecular structure of the
precursor will determine the shrinkage of the structural frame
and the possibility of micropore generation in the frame, and
therefore, the morphology and the SSA of the OMC are formed.
Commonly applied precursors can be categorized into those
with loose molecular structures such as sugar, sucrose and
furfuryl alcohol, and those with dense aromatic structures such
as pitch, pyrene, polyacrylonitrile, and acenaphthene. Using the
latter category of precursors, the OMC could replicate the
reverse image of the hard templates with minimal framework
shrinkage, high mechanical strength, and negligible micro-
porosity. In contrast, if precursors with loose structures are
applied, framework shrinkage will increase the mesopore size,
and particularly micropores will be generated in the frame-
work, leading to bimodal pore-size distribution and a larger
SSA. When an SBA-15 silica template is used, micropores in the
OMC can also be produced due to the micropores in the pore
walls of the template.28,29
Although silica is an ideal template for the preparation of
OMC, template removal is time-consuming and somehow destruc-
tive to achieve the complete removal of silica. Other mesoporous
templates can have some advantages. For instance, electroactive
materials are excellent templates if the target application of OMC
is in electrochemical systems. For instance, mesoporous nickel
oxide, which is an electroactive material for supercapacitors, has
been successfully utilized to prepare OMC.30
With the sacrifice of the template used, this hard-template
based strategy has its intrinsic limitation on cost. However, it
does have several prominent advantages. The impregnation
mechanism offers a relatively facile process to precisely replicate
the negative image of the hard template, and the nature of the
hard template ensures the pyrolysis process causing less damage
to the structure regularity and ordering. Another prominent
merit of this method is easier graphitization of the OMC formed
within the hard template.
2.3. OMC synthesis: soft-template based
Instead of sacrificing the template by etching it away, it is
possible to directly synthesize OMC by self-assembling a block
copolymer surfactant and a carbon precursor.4,31–35 The advantage
of this method is the absence of the template removal step, which
is somewhat destructive. An OMC with mesopores in the range of
3–7 nm can be easily synthesized by this method. The interaction
between the carbon precursor and the surfactant, which drives the
self-assembly of the soft template, determines the pore structure.
This strategy is rooted in the pioneering work on the M41S family
silica materials.13 The association of surfactant micelles with the
precursor through a weak interaction, such as hydrogen bonds,
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leads to the polycondensation of the precursor. The self-assembly
of the composite micelles yields an ordered mesostructured
carbon. The removal of the soft template and further carbonization
of the remaining precursor polymer yields the OMC with a defined
symmetry and pore size.
Since the early report of the soft-templated OMCs by a stepwise
assembly approach,31 great progress has been made in synthesizing
OMCs using this method, as has been comprehensively reviewed by
Yuan’s group.36 A variety of OMCs were synthesized in the forms of
spheres,37 rhomb-dodecahedra,38 wires39 and ribbons,40 films,31 or
monoliths.41 The strategy, through the supramolecular assembly
of the soft surfactant templates, can be accomplished by an
evaporation-induced self-assembly (EISA) or hydrothermal process.
The EISA of a block copolymer and resols is a facile approach with
flexibility since it can separate the cross-linking and thermo-
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polymerization process of the resols from the self-assembling
process. The ordered mesostructure is formed on the solvent
evaporating surface, and therefore, the OMC films could be
produced. Different OMCs with 2D hexagonal, lamellar, 3D
bicontinuous, body-centered cubic, and other structures have
been prepared using this route.42 Using water to replace the
organic solvents is an alternation,43 in which the surfactant-
driven self-assembly and carbon precursor polymerization occur
in a cooperative process. Such an aqueous route offers better
reproducibility and is suitable for large scale production. The
hydrothermal process was also reported to fabricate OMCs.37,41
Direct synthesis with surfactant recycling provides the
opportunity for large-scale production. The challenge of this
strategy is that currently available options of the soft templates
are mainly limited to block copolymers and the precursor to
phenolic resin. The block copolymer limits the minimum pore
size to ca. 3 nm. Smaller amphiphilic molecules as templates
should be explored for smaller pore sizes.
Upon comparing the OMCs synthesized from these two
strategies, it is found that the soft-template OMCs have thick
pore walls with a continuous framework, and thus, offer stability
in harsh thermal and oxidation treatments for functionalization.
However, the hard-template OMCs are much easier to be gra-
phitized, while it is difficult for the soft-template OMCs.
The morphology of the OMCs (including specific surface
area, pore size, and volume) can be altered by post-synthesis
modification. KOH activation is a common method industrially
employed for generating the micropores in activated carbon.2,44–46
Depending on the activation conditions (temperature, concen-
tration, etc.), the micropores generated can merge into each other
to form mesopores or create a microporosity texture. In the
latter case, micropores can build shortcut bridges between
the mesopores, which can be beneficial for electrochemical
performance.47 This method of activation can double the
specific surface area of OMC.
2.4. Graphitization of OMC
It is sometimes wrongfully suggested that OMC is not a
graphitic material. Considering the fact that amorphous carbon
materials are actually a form of disordered graphite, these types
of carbonaceous materials are always graphitic with different
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degrees of graphitization, which is usually judged by the D and
G bands in Raman spectra. From a practical perspective, the
OMCs with a higher graphitization degree are better for various
applications. This is particularly true for electrocatalyst and
electrode applications in which higher electrical conductivity
critically depends on the degree of graphitization.48 Thus, there
is demand for increasing the degree of graphitization of OMCs.
Low-temperature carbonization offers a well-ordered struc-
ture, but with an amorphous or low degree of graphitization
framework. Post-synthesis thermal treatment,49 particularly if
conducted at a high temperature (42000 1C), will induce
significant graphitization, but result in a lower degree of
ordering with broad pore-size distribution. Carbon precursors
with rich fused aromatic structures such as polyaromatic
hydrocarbons or aromatic molecules23,50–55 are better than
those with loose molecular structures since the former can be
graphitized at much lower temperatures, particularly when
an iron-based catalyst is incorporated.28,56 CVD growth at a
temperature higher than 900 1C is another option,57 leading to
the formation of graphitic OMCs.57–60 In almost all methods,
the reaction or treatment is conducted at a high temperature
where carbon atoms have enough energy to arrange or re-arrange
themselves into the graphitic hexagonal form.61 The temperature
could be lowered in the presence of catalytic species, particularly
iron-based nanomaterials.
A simple and effective approach is the carbonization of
metal phthalocyanines within an SBA-15 template.60 However,
this method is not practical because of the high cost of
phthalocyanines. It has been reported that phthalocyanine
can be replaced by natural fat as the carbon feedstock in the
same template system to produce the OMCs with graphitic
walls at relatively low temperature.62 A new approach is to
utilize a triblock-copolymer template, which results in the
formation of highly graphitic OMCs while the mesopore size
is strongly tunable in the range of ca. 3–40 nm.31,32,63,64
Graphitization of OMC is of particular importance in electro-
chemical systems, as it increases the electrical conductivity,
which is indeed a major requirement to reduce the charge transfer
resistance. In the absence of appropriate graphitic conductivity,
the electrical conductivity of OMC should be improved by some
conductive agents such as graphene or metals to achieve the
required conductivity for electrochemical performance.65–74
2.5. OMC with graphene walls
Graphene foam has been developed in recent studies of graphene-
based electrode applications. Chemically-derived individual
reduced graphene oxide sheets, with a sub-micrometer size,
can be assembled into a foam structure through freeze-drying
or similar methods.75–77 Such a graphene foam has irregular
pore distribution, and particularly, it does not form an
intimately connected network. Direct growth of multilayered
graphene (MLG) inside of a 3D metal frame resulted in macro-
pores of a few hundred micrometers in diameter by the metal
foam template.78 Both are not the optimized electrode struc-
tures when compared to the graphitized OMC structure with
graphene walls.

Materials Chemistry Frontiers
The OMC with graphene walls is a variation of graphitized
OMC when the highly graphitized pore wall is thinned down to
a few atomic layers. The soft-template based method will not
provide a high degree of graphitization and is therefore unsuitable
for producing graphitized OMC; while for the hard templates, in
order to obtain pore walls of graphitized OMC down to several
atomic layers, the void space in the hard templates should be thin
enough. Furthermore, the high degree of pore ordering and
graphitization demands a catalytic graphitization process at a
moderate temperature.
Jang et al.79 reported the growth of mesoporous graphene
balls (MGBs) using drop-cast polystyrene (PS) beads as a template.
As illustrated in Fig. 2a, carboxylated PS was synthesized via
emulsion polymerization and then sulfurized to obtain SPS-COOH,
which can strongly absorb iron ions (Fe3+) when immersed in
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FeCl3 solution. Using the drop-cast beads as templates and pre-
cursors, the sample was annealed in an H2/Ar environment to
catalytically promote graphene ball growth. Thus, the resulting
graphene balls have a diameter similar to the functionalized PS
beads, but etching away the Fe from the sphere walls will form
MGBs, as shown by the transmission electron microscopy (TEM)
images in Fig. 2b and c. Due to the irregular distribution of the PS
beads in the template, the synthesized MGBs did not form an
ordered 3D macrostructure.
Dong et al.22,80 took one step further to synthesize graphitized
OMCs with superlattice symmetry. In their work, the Fe3O4
colloidal NPs formed a superlattice structure, which was
employed as both the template and the catalyst. Using oleic acid
(OA) capped Fe3O4 colloidal nanocrystals (NC), a 3D superlattice
was self-assembled followed by the carbonization/graphitization
of the OA ligands at 500 1C in the presence of an iron catalyst.
Fig. 2 (a) Schematic of mesoporous graphene nanoball synthesis from
drop-casting a functionalized bead/FeCl3 solution, to thermal annealing
for graphene growth, and etching away the Fe domain. (b and c) TEM
images of the mesoporous graphene nanoballs. Reproduced with permis-
sion from ref. 79. Copyright 2013, American Chemical Society.
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The partially graphitized OMC after the NC removal is shown in
Fig. 3a and b. Further heat treatment at 1000 1C results in the
formation of multilayered graphene as a pore wall (Fig. 3c and d).
The resulting graphitized OMC exhibits a long-range highly-
ordered superlattice symmetry, replicated from the template.
Huang’s group81 employed SBA-15 as a template and poly-
furfuryl alcohol (PFA) as a precursor to synthesize a graphitized
OMC. Fig. 4 demonstrates the synthesis procedure. First, an
impregnated template is formed by depositing the Ni agent
within the silica template, and then the N-doped ordered
mesoporous with walls made of few-layer carbon are built
within the template using a CV process. The final step is the
removal of the template and the metallic catalyst.
2.6. Graphene edge-oriented pore walls
For these highly graphitized OMCs, the graphite basal plane is
generally exposed as the pore wall surface. In electrochemical
Fig. 3 (a) Schematic of OMG synthesis from colloidal Fe3O4 NPs. (b and
c) TEM images of the as-synthesized OMC superlattice after catalytic
carbonization at 500 1C with fcc symmetry. (d and e) TEM images of
OMG after being further graphitized at 1000 1C, imaged for the (111) plane.
Reproduced with permission from ref. 22. Copyright 2015, Wiley-VCH.
Mater. Chem. Front., 2017, 1, 1001--1027 | 1005
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Fig. 4 (a) Schematic of synthesizing nitrogen doped OMG. (b) Low-angle X-ray diffraction patterns of the synthesized sample with or without N-doping,
showing the characteristic peaks of hexagonal packing. Reproduced with permission from ref. 81. Copyright 2015, American Association for the
Advancement of Science.

systems, the graphite basal plane is far less attractive than the
edges. Ideal graphene is not an interesting material in terms of
electrochemical reactions due to the high ratio of the basal
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plane to edges, and particularly the flatness of the hexagonal

network of carbon atoms in which the sp2 hybrid is not very
reactive.82 The latter is somehow shielded by the p electrons
avoiding direct adsorption at carbon atoms. It is known that the
edge plane of highly oriented pyrolytic graphite has an electro-
chemical reactivity several orders of magnitude higher than its
basal plane due to a large amount of defects, such as kinks,
steps, and vacancies, at the edge that produce a high density
of defect states near the Fermi level.83 These atomic edges or
steps are the potential adsorption sites of redox species in the
electrolyte and sites of electron transfer. The edge planes can
also provide an electrical double layer capacitance of 50 to
70 mF cm 2 in comparison with that of basal planes, which
provide a capacitance of only B3 mF cm 2.84 The edge-oriented
multilayered graphene flakes have been investigated for a variety of
Fig. 5 (a) Schematic of CMK-3G OMG consisting of hexagonal arrays of
electrochemical applications.85–88 Therefore, it is highly desirable
carbon nanorods, while the nanorods are formed by stacking of the
to synthesize OMCs with exposed graphene edges. discoid graphene sheets oriented perpendicular to the rod orientation.
Using Al-incorporated silica templates and various aromatic (b) TEM images of CMK-3G showing the rod array. (c) TEM images showing
compounds as precursors in an autoclave process, followed by the stacked discoid graphene sheets. The inset shows the corresponding
further graphitization at high temperatures, Ryoo’s group56 electron diffraction pattern. Reproduced with permission from ref. 84.
Copyright 1971, The Electrochemical Society.
demonstrated a unique CMK-3 OMC with graphitic framework
structures through in situ conversion of the aromatic com-
pounds into mesophase pitch inside the silica templates. However, our knowledge about the arrangement of graphene
The degree of graphitization of OMC can be at the level of hexagons across the mesopores is very limited. In the graphene
multi-walled carbon nanotubes or multiple-layer graphene. A structure, edge atoms have anomalous electronic properties
striking feature is that the hexagonal arrays of carbon nanorods resulting in different electrochemical performance. However,
are formed by stacking of the discoid graphene sheets oriented the actual atomic structure of the edges of OMC mesopores is
perpendicular to the rod orientation, with the exposed edge-on not fully understood.
graphitic structure, as shown in Fig. 5.
Utilizing nickel foam89 or cellulose paper90 as a template,
Ren et al. deposited an edge-oriented multiple-layer graphene 3. OMC in electrochemical systems
porous structure using a plasma CVD process and the template
can be removed.91 Since the template used has large pores 3.1. Electrochemistry of OMC
without ordering, the edge-oriented graphene porous structure A comparative study revealed that the electrochemical activity
thus produced does not belong to the category of graphitized of the OMC is higher than that of graphene, which is a popular
OMC. However, if suitable templates are used, such a plasma material in the realm of electrochemistry.92 In a sense, OMC is
CVD process may provide a viable approach for producing edge- considered as an alternative to the classical microporous carbon
oriented graphitized OMC. materials which have been commercially available for decades.
In general, there are various methods to enhance the degree Therefore, the goal of OMC production is to achieve the highest
of graphitization of the OMCs to align the p electrons along the possible specific surface area, but this is not the main requirement
ordered architecture, and it is still an active area of research. in the electrochemical systems. Microporous carbonaceous

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materials have an extremely high specific surface area, but
micropores are too small for the diffusion of electroactive
species. Since mesopores fit well with the size of diffusing
species, OMCs have attracted considerable attention in the
realm of electrochemistry. However, the common standpoint
was to employ the OMC as a high surface area carbon. This is
the reason that the majority of electrochemical studies of OMCs
are focused on supercapacitors93–105 or sensors.106
The characteristic feature of the OMC in electrochemical
systems is the possibility of fast diffusion through the solid
electroactive material. Unfortunately, our understanding of the
electrochemistry of OMCs is very limited, as fewer efforts have
been made for this important issue. There is a similar situation
for the electrochemistry of graphene because graphene is not
as simple as the flat hexagonal network of carbon atoms
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is of particular importance for electrochemical systems.
Ordered hierarchical mesoporous/macroporous carbon dis-
plays good performance in electrochemical systems, as the
ordered macropores facilitate fast diffusion through the elec-
trolyte to mesopores.113 Fig. 6 shows the ordered structure at
two different scales of such carbonaceous materials.
Fig. 7 displays how a macroporous structure can be created
using mesoporous building blocks. Such two-level porous
carbon has been prepared using different methods.114 A
simple idea is to use two different templates for the formation
of macropores and mesopores simultaneously. For instance,
polystyrene is known as a good template for the formation
of macropores; introducing silica nanoparticles creates
mesopores throughout the walls of the macroporous carbon
synthesized.115

imagined.107–109 Instead, graphene is full of chemical and

physical irregularities which can substantially change the 3.3. OMC nanocomposites
electrochemical process. This misleading comes from the As described above, OMC is prepared to utilize mesoporous
straightforward structure of ideal graphene, but OMC chemical templates, which should be removed. Depending on the pro-
irregularities are too complicated even for an ideal structure. perties of the template, the final material can be OMC/silica,
The arrangement of carbon atoms at the mesopore edges is which is indeed a nanocomposite with potential applications.
indeed a mystery, particularly as the graphitization level of In a similar fashion, OMC can be used as the template for the
OMC is not absolute or uniform. Similar to graphene, the synthesis of a mesoporous electroactive material; then, it is not
electrochemistry at the mesopore edges is completely different necessary to remove the template, as the OMC template is
from that on the internal walls of the mesopores. A key indeed an important component of the targeted nanocompo-
difference is that edges and dangling atoms in graphene are site. This leads to the formation of a uniformly distributed
chemically preferred sites; but in OMC, the mesopore edges
are even physically preferred to initiate the electrochemical
reactions, as they are more accessible.
Since carbonaceous nanomaterials are subject to chemical
treatment resulting in severe structural changes, their electro-
chemistry cannot be easily judged. For instance, it was claimed
that the majority of the electrochemical activity of graphene
samples is due to the defects formed during the post-treatment
rather than the original graphene structure.110,111 This phenom-
enon is more complicated for OMC, as the template removal is at
the atomic scale. In other words, not only the chemical treat-
ment but also the carbon template interactions can result in
peculiar defects.
Electrochemistry within the OMC matrix is probably different
from that on other carbonaceous nanomaterials and far from
fully understood. For instance, double layer capacitance is a
straightforward phenomenon with least electrochemical com-
plexity, but the specific capacitance of OMC within its silica
template is similar to that after template removal.112

3.2. Micropores within macroporous structures

The internal accessibility of mesopores is not the only factor in
electrochemical performance, as electroactive species should
reach the mesopores regularly. Since the rate-determining step
in most electrochemical systems is the diffusion process, it is
vitally important to facilitate fast diffusion of electroactive
species to keep them ready for insertion into the mesopores.
Note that the charge transfer resistance for a conductive carbon Fig. 6 SEM and TEM images of an ordered hierarchical mesoporous/
with a high specific surface area is not normally the rate- macroporous carbon at different scales. Reproduced with permission from
determining step. This macrostructure of mesoporous carbon ref. 113. Copyright 2013, Wiley-VCH.

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Fig. 7 An illustration for designing carbon-supported Pt electrocatalysts with macroporous/mesoporous architecture. Reproduced with permission
from ref. 114. Copyright 2015, Wiley-VCH.
nanocomposite, which is indeed a key goal for electroactive
nanocomposites in which carbon should contribute to the
electrical conductivity and fairly separating the electroactive
materials to become more electrochemically accessible. OMC
has been widely used as a nanocomposite component for various
electroactive materials.116
Since the size of the mesopores is too small for conducting
uniform reactions therein, it is a serious challenge to uniformly
fill the mesopores with the second component. For instance,
sonochemical synthesis can result in a more uniform distribu-
tion of reactants to form the electroactive material uniformly
distributed over the OMC pores.116
A common issue for electroactive materials is the necessity
of binders to form a solid electrode. Binders are usually
electrochemically inactive and may block the diffusion of
electroactive species; besides the fact that their mass reduces
the specific energy and power of electrochemical power
sources. In addition to the possible chemical interaction of
OMC with electroactive materials, the interconnected architec-
ture of OMC provides a rare opportunity for in situ preparation
of nanocomposites in which the electroactive material is
entangled through the OMC scaffold.117,118
While OMC mesopores can serve as local tubes for the
formation of an electroactive material, micropores are too small
and will be blocked by the resulting material for electrochemical
performance.119 This blockage is not necessarily physical filling,
as mesopores are also filled with the electroactive material, but
its lattice network is still large enough to allow solid-state
diffusion. This feature is not limited to OMC, and 3D MCs with
larger mesopores are indeed good matrices for the formation of
electroactive materials.120
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4. OMC in electrochemical energy
storage
4.1. OMC for ultracapacitors (double layer capacitors)
High surface area carbon has always been the first choice for
double layer capacitors (aka ultracapacitors). It is not difficult
to prepare a carbon with an extremely high surface area, but not
all the surface area is electrochemically accessible. Thus, most
carbon-based ultracapacitors have specific capacitance below
their theoretical capacities. OMC can provide an ordered matrix
for the interfacial interaction with charged ions within the
electrolyte solution. However, the limitation is the size of the
mesopores. If they are too small, ions cannot freely diffuse
therein, and if too large, the specific surface area is low. In fact,
the mesopores should be tuned for a specific ultracapacitor
depending on the size, charge, and structure of the electro-
active species forming the double layer.121 Gogotsi and Simon
have elaborated the dependency of the specific capacitance
of an OMC on the pore size.122 In general, an OMC with suffi-
ciently large pores has a specific surface area around 1000 m2 g 1,
resulting in specific capacitance comparable with other types
of carbon materials.65,123,124
However, the capacitive behavior of OMC is not straight-
forward as the nature of the double layer within the mesopores
is still ambiguous. Different values have been reported for the
specific capacitance of similar OMCs. It has been explained
that the synthesis conditions and post-treatment have huge
impacts on the electrochemical performance of OMC.125
Highly ordered single crystals of mesoporous carbon show
excellent electrochemical performance for ultracapacitors.126
The large crystalline particles dictate that the electrochemical

Materials Chemistry Frontiers
process is conducted through the particle matrix rather than
the external interface (Fig. 8). Although it is not entirely a solid-
state system because electrolytes are soaked within the meso-
pores, the electrochemical performance relies on diffusion
through interconnected pores. This clearly indicates that inter-
nal mesopores are responsible for the high specific capacitance
achieved (281 F g 1 at 0.5 A g 1 in a 6 M KOH electrolyte) rather
than having a high surface area because of smaller particles.
The importance of this feature is because of the essential
requirement of the electroactive packing within the electrode
structure. It seems that larger particles, which are of practical
interest, with mesoporosity, can provide a large electrochemi-
cally accessible area. However, it should be taken into account
that the cyclic voltammetric behavior indicates that the system
is not purely capacitive. In addition to the complicated pseudo-
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capacitive contribution, the solid-state diffusion is a rate-
determining step when the electrochemically accessible area
is mostly spread through the internal mesoporosity.
The important feature is that the well-ordered particle
morphology does not guarantee a smooth electrochemical
performance. Two different factors are responsible for this
deviation from an ideal behavior. (i) The diffusion of electro-
active species within the mesopores, which is dependent on the
uniform distribution of the electrolytes within the mesopores
and how the mesopores are interconnected. (ii) The macro-
structure of the electrode in which the individual particles are
packed together. Although the inner structure of the OMC
might be well-oriented, there is still no guarantee that the
mesopores are electrochemically accessible. In the material
characterization, the mesopores might seem open in TEM
images, but when packing the particles, some mesopores are
blocked by the neighboring particles. Therefore, the ordered
structure whether at the mesoscale or larger scales cannot be
the sole basis for the material performance, instead, the
electrochemical accessibility should be inspected at different
scales.
Fig. 8 (a–h) SEM and TEM images of an N-doped OMC with Im3m symmetry and rhombic dodecahedral single crystal morphology. (i) Cyclic
voltammograms and (j) charge/discharge profiles of the N-doped OMC as an ultracapacitor. Reproduced with permission from ref. 126. Copyright 2015,
Royal Society of Chemistry.
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The best capacitive behavior of OMC is obtained when the
degree of graphitization is maximum.127,128 Since the graphene
basal plane is not electrochemically active,110,111 the formation
of graphitic walls along the 001 direction assists charge transfer
between the electrode/electrolyte interface and the current
collector. Furthermore, the shape and the structure of the
double layer over the basal plane of graphene are different
from those on amorphous walls of mesopores.
The unique feature of OMC is the translational symmetry
of its unit cell, but the internal structure of the unit cell of
mesopores can have a rough texture. Although micropores
are too small for long diffusion of electroactive species, the
presence of microporous texture on the walls of mesopores can
be beneficial for ultracapacitor performance as far as they are
accessible.129,130
Highly ordered nanofibers of OMC provide an architecture
for more effective diffusion of the electroactive species across
the electrode matrix. OMC nanofibers display a well-defined
capacitive behavior.131 On the other hand, as the nanofibers
can be prepared using an AAO hard template, it is possible to
directly grow them on the current collector, which is in favor of
the overall electrical conductivity and suitable for high-power
micro-supercapacitors.132 The hollow structure can provide a
better accessibility of the mesopores from both sides, and the
specific capacitance of a fibrous-structured hollow OMC has
been reported to be very high (359 F g 1), with an extremely
large power density (10 kW kg 1) in a 6 M KOH electrolyte.133
In a similar fashion, OMC can be directly synthesized on a
polymer substrate to form a flexible film.134 It is a general
demand to make the electrochemical cells flexible for wearable
electronics, which is realistic by the development of gel electro-
lytes; however, electrode materials are usually fragile, and the
main obstacle still exists in this direction.
The superiority of OMC for supercapacitors is not limited to
its high surface area. It is well known that a purely double layer
capacitor based on the carbonaceous material is not realistic,
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as there are always some faradaic redox reactions. This is
primarily because of the functional groups formed or adsorbed
on the active surface of the carbon. This behavior is more
studied for the functional groups on graphene, particularly
chemically-derived reduced graphene oxide,135–137 but similar
mechanisms are also applied to surface-modified OMC. The
presence of various functional groups can significantly alter the
electrochemical performance of OMC.138 Chemical treatment
or activation of OMC results in the formation of such functional
groups, which are responsible for part of the superior ultra-
capacitor performance.139
Similarly, graphene edges play particular roles in electro-
chemical systems, as the charge transfer mechanism and
barrier can be utterly changed through the dangling bonds at
kinks, steps, and vacancies at the edge that produce a high
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density of defect states near the Fermi level.140 Therefore, the
graphite edge plane offers a capacitance 20 times larger than
the basal plane. This feature can also be the case for OMC pores
having sharp edges. Nevertheless, the structural arrangement
of carbon atoms in OMC has not been fully understood yet. The
peculiar charge transfer can be controlled by the morphological
structure or degree of graphitization of OMC.
Similar to the role of functional groups, doping alters the
uniformity of charge distribution across carbon atoms, and
chemical reactivity to have more contributions of pseudo-
capacitive nature. Nitrogen is the most common element for
the doping of various types of carbon materials, which also
enhances their electrical conductivity. It has also been widely
used for the doping of OMC.141–150 Owing to the pseudo-
capacitive contribution, the specific capacitance of N-doped
OMC is over 300 F g 1 in a 1 M H2SO4 electrolyte.151
Another important feature of doping is to enhance the
wettability of OMC, which is a serious requirement for ultra-
capacitors, and also other electrochemical applications. Pristine
OMCs normally have a hydrophobic nature, and thus, the
electrode/electrolyte interface is poorly formed. N-doping can
scientifically contribute to the surface polarity of OMC, but it is
not easy to dope a high content of nitrogen. The presence of a
Pluronic surfactant having a high content of oxygen in the OMC
synthesis interacts with an N-rich carbon precursor to decom-
pose it. This results in a deformed mesostructure, and thus,
N-doping sacrifices the uniformity and order of OMC.152–154 On
the other hand, simply increasing the amount of nitrogen dopant
is not beneficial for the ultracapacitor performance. Although
nitrogen doping generally increases the electrical conductivity of
carbon because of a higher charge/electron carrier mobility,155,156
too much N can increase the interfacial resistance too.157 More-
over, the pseudocapacitive process contributed by the presence of
N can block the original double layer capacitance (because the
electrode surface does not have a uniform charge distribution for
the formation of the classic Helmholtz layer), resulting in a
smaller overall specific capacitance. A comparative study showed
that the optimum amount of N doping for an OMC ultracapacitor
is about 6%.157
In any case, N-doping can significantly improve the specific
capacitance of OMC-based ultracapacitors.155,158–164 The surface
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of the mesoporous silica template plays a substantial role in
the chemical structure of OMC, and can result in the formation
of an N-rich surface having a significant redox system. This
significantly improves the electrochemical performance.158 The
presence of N adatoms and surface groups paves the way for new
faradaic reactions, which can contribute to the pseudocapacitive
performance, e.g. by facilitating H insertion.165 The specific
capacitance of an OMC-based ultracapacitor can be directly
increased by increasing the presence of nitrogen while the
presence of oxygen functional groups has a slight influence.166
Although the role of the N dopant is to cause chemical
inhomogeneity, its influence depends on the OMC architecture
too. This effect is much higher for a 3D architecture of OMC
(e.g. FDU-16), as the specific capacitance is increased 7 times by
N-doping.167 While the original FDU-16 OMC is not considered
as a promising material for ultracapacitors, N-doped FDU-16
OMC is among the best candidates. The cyclability is impress-
ive, as the specific capacitance actually increases during the
first 10 000 cycles due to the structural rearrangement opening
new channels for diffusion.167
Another common dopant of carbon is boron.168 Doping of
OMC with boron also increases the specific capacitance.169
When substituting carbon, boron atoms are natively bonded
with oxygen atoms. The change in charge distribution across
the carbon network and the oxygen functional groups directly
bonded with the OMC lattice causes a significant contribution
of pseudocapacitance in addition to the original double layer
charging.170 Nevertheless, this chemical reactivity results in
poor cyclability due to structural changes in the course of
faradaic reactions.170
While neighbor elements (B and N) just alter the uniformity
of charge distribution across the carbon network, doping
with larger elements such as P can alter the morphology too
resulting in substantial changes in the surface area and pore
volume.171
While hydrophilicity can improve the electrode wettability in
electrochemical systems, hydrophobicity can reduce corrosion.
Doping of OMC with P increases the hydrophobicity, and thus,
protects against corrosion.172 Sulfur functional groups can also
contribute to the pseudocapacitive behavior of OMC.173 This
also emphasizes that the influence of doping is not only due to
the presence of the doping element in the carbon network
(changing the charge distribution) but also the functional
groups formed on the dopant.
In fact, while the uniform architecture of OMC is beneficial
for electrochemical performance, chemical uniformity is not
desirable, because chemical inhomogeneities of atoms at the
electrolyte/electrode interface facilitate charge transfer and
electrochemical reaction. While gaining the ordered structure
of OMC, doping can create chemical inhomogeneity. Increasing
this inhomogeneity with multiple dopants can significantly
increase the specific capacitance, e.g. N/P,171,174,175 B/P,176
and N/S.177–180
Although the large surface area provides a significant double
layer capacitance, the faradaic pseudocapacitance (or more
precisely a pseudocapacitive mechanism) of N-doped OMC is
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becoming dominant at high dopant concentration.181 There-
fore, the impedance spectroscopic spectra of N-doped OMC
represent the characteristics of faradaic systems with a charge
transfer semi-circle followed by Warburg impedance.
An important issue, which is usually neglected, is the
electrolyte solution. It is evident that the capacitive behavior
is affected by the electroactive species due to their charge, but
the influence of size is of critical importance for OMC, as
the sizes of hydrated/solvated ions are comparable with
those of mesopores. This means that some ions are larger or
smaller than OMC mesopores, leading to different capacitive
behaviors.182,183
It is worth emphasizing that a nitrogen-doped nano-tubular
ordered mesoporous few-layer carbon (OMFLC) structure81 has
a large surface area (1580 m2 g 1), a large total pore volume
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specific surface area; thus, a significant fraction of the faradaic
reaction occurs at the surface with no need for slow solid-state
diffusion to reach the reactive redox sites, with the latter being
characteristic of charge storage in a battery.
Transition metal oxides are the common candidates for
pseudocapacitors. Due to their electronic insulating nature,
carbon nanostructures are commonly used as a conductive
framework for these electroactive oxides. Increasing the specific
surface area is indeed a common strategy in developing electro-
active materials for supercapacitors. High surface area nanocom-
posites with carbon are an appropriate design, as nanostructured
carbon can assist in distributing the electroactive material while
contributing to the electrical conductivity. In addition to common
advantages of carbonaceous nanomaterials, OMC can serve as an
ideal template for the formation of a nanostructured electroactive

(2.20 cm3 g 1), and an average pore width (2.25 nm). After
composition optimization, a specific capacitance as high as
855 F g 1 at a current density of 1 A g 1 was obtained in an
aqueous solution of H2SO4 (Fig. 9a and b). The Ragone plot of
energy vs. power densities of symmetric cells based on this
material in two different electrolytes (H2SO4 and Li2SO4) shows
extraordinary performance compared to other conventional
batteries and supercapacitors (Fig. 9c and d).
4.2. OMC for pseudocapacitors
In pseudocapacitors, the so-called pseudocapacitance is the
result of facile faradaic redox reactions at the surface or sub-
surface of the electroactive material. Better rate capability and
pseudocapacitive behavior are obtained when the ratio of surface
reaction is significant in comparison with that of the solid-state
reaction. This dominance can be formed by increasing the
material. Because of inter-connections of OMC pores, the electro-
active material is widely exposed to the electrolyte to shorten the
diffusion paths by minimizing solid-state diffusion.184
OMC can chemically interact with the precursors for in situ
synthesis of the electroactive nanocomposites.185 This is
obviously accompanied by higher mechanical stability and elec-
trically conductivity. Owing to the mechanical stability of elec-
troactive materials within the OMC architecture, supercapacitors
based on OMC nanocomposites show practical cyclability over
thousands of cycles.186
Conductive polymers are good candidates for supercapacitors,
as their redox systems are normally spread over wide ranges of
potentials delivering pseudocapacitive behavior. Although diffu-
sion through the polymer matrix is not very slow, it is still necessary
to reduce the solid-state diffusion. Interestingly, monomers can be
injected within the OMC mesopores to initiate the polymerization

Fig. 9 (a) Cyclic voltammetry test and galvanostatic test of the cells using different components. Ragone plot of specific energy vs. specific power in
(c) and energy density vs. power density in (d) of the cell performance, in comparison with other conventional batteries and supercapacitors. Reproduced
with permission from ref. 81. Copyright 2015, American Association for the Advancement of Science.

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from within the pores.187 Electrochemical polymerization of aniline
has also been conducted within the graphite interlayers.140 The
specific capacitance of OMC/polyaniline can be over 900 F g 1 with
an excellent cyclability over thousands of cycles in a 1 M H2SO4
electrolyte.187 OMC/polyaniline shows a good mechanical stability
because of molecular interactions within the nanocomposite
matrix.188 It has been shown that the rate capability of an
OMC/polypyrrole supercapacitor is about 50% better than pure
polypyrrole.189 The OMC/PEDOT supercapacitor showed only
14% capacity loss after 10 000 charge/discharge cycles.190
The conductive polymer formed within the 3D meso-architecture
of OMC can be the matrix for additional electroactive materials too.
The interesting feature is that all the reactants can chemically
interact for designing an in situ synthesis. For instance, polyaniline
and manganese oxide directly synthesized within OMC showed
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a good supercapacitor performance.191–193 An extremely high
specific capacitance of 1668 F g 1 has been reported for ruthenium
oxide/iron oxide embedded within OMC in a 0.5 M H2SO4
electrolyte.194 In general metal oxides embedded in OMC display
high specific capacitance.195
It should be taken into account that the size of mesopores is
somewhat comparable to the lattice size of the electroactive
material. Thus, the presence of an appropriate amount of
reactants within the mesopores is highly effective. For the case
of metal oxide, the size, shape, and charge of the reactant anion
play a substantial role in the structure and pseudocapacitive
behavior of the metal oxide formed within the OMC.119
Comparison of 1D, 2D, and 3D OMCs made from different
templates revealed that the ion mobility significantly depends
on the diffusion direction in an OMC/Fe2O3 nanocomposite. 1D
architectures showed the best rate capability in electrochemical
performance, probably because of fewer interactions between
the diffusing species.196
The presence of nitrogen heteroatoms in the structure of
OMC can significantly improve the interaction with electro-
active materials resulting in enhanced specific capacitance.197
4.3. OMC for lithium ion batteries
The important roles of carbonaceous materials whether as
active materials or conductive agents in both anodes and cathodes
of lithium ion batteries are evident. On the other hand, knowing
the fact that the main challenge of lithium batteries has always
been related to the slow solid-state diffusion, the ordered inter-
connected channels of OMC can provide a new opportunity.
Most of the electrode materials of lithium ion batteries are
poorly conductive. Carbon is a good conductive agent, but it also
blocks the Li diffusion. For instance, LiFePO4 is a promising
cathode material, but it needs a conductive agent to reach an
acceptable conductivity for charge transfer from the redox sites
to the current collector. LiFePO4/OMC has been synthesized by a
one-pot route.198 In this direction, OMC paves the way for
employing novel candidates, which are not practical standalone
systems.199 The 3D structure of OMC is an excellent matrix for
the inclusion of electrode materials for battery performance.200
Synthesizing hollow OMC does not result in a high specific
surface area (usually in the order of 500 m2 g 1), but as the
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outer structure has a better electrochemical accessibility, the
material displays a high rate capability for lithium ion batteries
by reducing the struggles of the Li cation in solid-state
diffusion.201,202
The OMC scaffold provides an excellent matrix for the
preparation of electroactive nanocomposites as both anode203–207
and cathode198,199 materials. The majority of these nanocompo-
sites are prepared by in situ pore-filling approaches. In this case,
the material density and mechanical stability are high enough for
practical applications.
In this direction, the OMC architecture is of key importance,
as the diffusion of Li-ions is the rate-determining step. The
lithium battery performance of Sn nanoparticles embedded
within an OMC with larger pores and thinner pore walls has
been reported to be better.160
Most of the OMCs are prepared based on silica templates,
and the template removal can be a harmful process. Quite
interestingly, silica is a promising candidate as an anode
material in lithium ion batteries; and preparation of silica/
carbon nanocomposites is an effective approach to overcome
the low electrical conductivity of the silica component. This
suggests that the OMC and its template can be active anode
materials for lithium ion batteries.208 In other words, this is
indeed an in situ synthesis of a highly ordered nanocomposite.
Pure OMC can be a candidate for anode materials similar to
other graphitic carbon nanomaterials. However, the electro-
chemical performance is significantly poor in comparison with
conventional graphite in which Li can be intercalated.209
In fact, although diffusion through mesopores is facilitated,
intercalation within the carbon lattice is not favorable in the
case of OMC.
In a similar fashion, OMC can be used as an electrode
material for other metal ion batteries. For instance, N-doped
OMC has been utilized as an anode material in sodium ion
batteries.210
4.4. OMC for metal–sulfur batteries
Metal–sulfur batteries have recently attracted considerable
attention due to their high specific capacity resulting in an
incredibly high energy density. The main challenge of these
types of batteries is the sulfur cathode. Since sulfur is non-
conductive, the cathode should be prepared using a conductive
agent. Like similar battery systems, carbon is the first choice as
the conductive agent, and various forms of carbon have been
employed for the fabrication of Li–S cathodes.211–214 Octasulfur
(cyclo-S8) is the common allotrope of sulfur, and its reduction
to the final product of Li2S during the discharge process is a
stepwise process, producing Li2Sn (n = 4–8) polysulfide inter-
mediates which are dissoluble in the electrolyte. The dissolved
polysulfides shuttle between and react on the sulfur cathode
and the lithium anode, resulting in a ‘‘chemical shortcut’’
inside the cell.215 This shuttle phenomenon causes irreversible
loss of active materials, capacity fade, self-discharge, and anode
etching, among many other detrimental effects. This is the
most formidable challenge for the sulfur cathode. Nazar and
her coworkers prepared OMC/S as a promising cathode
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material for Li–S batteries for the first time in 2009.216 The
interesting feature of this idea is that sulfur can be entrapped
within the OMC structure if the pores are of the right size. This
work started a new era in developing Li–S batteries by physically
trapping and chemically binding polysulfides in the cathode
matrix.
The point is that OMC provides a good permeability for the
electroactive species; thus, sulfur can be incorporated within
the OMC structure.217–219 This protects sulfur from dissolution
while keeping it electrochemically accessible. It is evident that
the key challenge for improving the battery performance of
OMC/S cathodes is to control the morphology to increase the
amount of sulfur entrapment. In general, OMC particles of
200–500 nm with mesopores of 3–10 nm have shown good
battery performance with specific capacities over 1000 mA h g 1.
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The OMC scaffold can retain a high amount of sulfur,

ca. over 50% therein.220 Owing to the mechanical stability of
entanglement within the interconnected mesopores, the OMC
cathode displays an excellent cyclability. Since sulfur is not a
concrete electrode material with a rigid structure like metal
oxides, it is subject to severe dissolution. The size of OMC
mesopores well fits with the S8 structure formed therein, and
thus, the OMC/S cathode shows an excellent cyclability in
comparison with other carbonaceous materials.221 However,
the performance is not straightforward in practice, as the
irreversible inclusion of sulfur within the microporosity of the
mesopores results in severe capacity fading. As a matter of fact,
OMC can be a good candidate as an S electrode if its architec-
ture is thoroughly designed.
In addition to physically entrapping polysulfides to retard
their diffusion out of the cathode, to further prevent the release
of sulfur, binding these polar species chemically onto the
carbon matrix is another strategy. Since carbon itself is intrinsically
non-polar with a lower binding capability to the polar polysulfides,
surface functionalization of OMC, including heteroatom doping,
conductive polymers or transition metal oxide and sulfide decora-
tion can dramatically enhance the binding capability of OMC to
polysulfides.222 With a surface of S-embedded OMC covered by a
conductive polymer, a high specific capacity over 1000 mA h g 1
is achieved with an acceptable capacity retention for over
1000 cycles.223 Using PEDOT decorated ordered mesoporous
carbon nanocubes to load sulfur, Wang et al.224 demonstrated a
sulfur cathode with large capacity, long cycling stability and
high rate capability (Fig. 10).
4.5. OMC for Li–air batteries
In metal–air batteries, such as Li–O2, the key challenge is the
porous catalytic cathode material in which Li2O2 is formed and
decomposed. It forms the bottleneck since the sluggish ORR/OER
kinetics increase the overpotential and limit the recharge capacity
and rate performance. The insoluble discharge product (Li2O2)
will gradually block the flow of the electrolyte and O2. It has been
demonstrated that the OMC skeleton is suitable for the formation
of Li2O2.225 The ordered matrix of OMC provides an opportunity
for uniform distribution of catalyst nanoparticles. This is of
particular importance, as metallic nanoparticles should not block
Fig. 10 (a) Schematic of PEDOT decorated mesoporous carbon nano-
cubes for a sulfur cathode. (b) Cycling performance at 0.5C and 5C, and
the corresponding Coulombic efficiencies. Reproduced with permission
from ref. 224. Copyright 2015, Elsevier.
the Li diffusion, which is the main charge carrier. Using an
ordered hierarchical mesoporous/macroporous carbon, a high-
performance cathode was demonstrated.113
The cathode of metal–air batteries resembles fuel cells
and needs ideal electrocatalysts for both the oxygen evolution
reaction (OER) and oxygen reduction reaction (ORR) during the
charge and discharge processes, respectively. Whether employ-
ing the classical Pt catalyst or a new alternative such as metal
oxides,226 a key requirement is a uniform distribution of the
catalyst over the catalyst support to make the catalyst more
accessible electrochemically. Using OMC as an electrocatalyst
will be summarized in Section 4.6. Wang et al. fabricated a
three-dimensional ordered mesoporous carbon by growing
a thin layer of FeOx using atomic layer deposition; when
decorated with Pd nanoparticle catalysts, the new cathode
exhibits a capacity greater than 6000 mA h g 1 and a cyclability
of more than 68 cycles.225 Fig. 11 shows the morphological
structure and the performance of the OMC/FeOx/Pt electrode.
Although the current focus is on Li–O2 batteries among
metal–air batteries, the possibility of employing OMC is not
limited to Li–O2 only. For instance, OMC has been successfully
employed for other metal–air cells such as Zn–air cells.227
4.6. OMC as an electrocatalyst support
Electrocatalysts participate in electrochemical reactions by low-
ering the reaction activation energy and by lowering the excess
energy consumed by the activation barrier. They play critical
roles in electrochemical fuel (H2, CO, CH4, etc.) production
and energy generation (e.g. in fuel cells). A wide range of

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Fig. 11 (a) Schematic of the catalyst loaded OMC structure. (b) Pore size
distribution change after FeOx coating. (c) TEM images of pristine OMC,
after FeOx coating, and after Pd NP decoration. (d) Schematic illustrating
the influence of Li2O2 deposition on the ORR activity of carbon and the
subsequent effects of the FeOx coating and Pd NP decoration. (e) Cycling
curves for the bare, FeOx coated, and Pd-decorated OMC electrodes.
Reproduced with permission from ref. 225. Copyright 2015, Wiley-VCH.
electrochemical systems have utilized Pt or similar precious
metals or transition metal oxides as electrocatalysts. The role of
the catalyst support is critically important in these systems to
fairly disperse the catalysts to improve the system efficiency and
reduce the amount of expensive catalyst required. Carbon is
an ideal catalyst support because of its electrical conductivity
and high specific surface area, and the mesoporous structure is
the best choice for two reasons: simultaneous synthesis of the
catalyst can result in the formation of uniform nanoparticles
over the mesopores as a template, and catalyst nanoparticles
can be uniformly distributed over the mesoporous structure. How-
ever, preparation of carbon/catalyst nanocomposites is not as easy
as it seems; a significant part of the catalyst is actually covered by
carbon and becomes electrochemically inaccessible.228,229
A preliminary study showed that the capability of OMC for
dispersing Pt nanoparticles is higher than those of similar
carbon nanomaterials.230 This named OMC as a promising
catalyst support for various applications, particularly fuel cells.
The morphology of micropores is basically responsible for the
desirable arrangement of metallic catalysts to be well dispersed
while electrochemically accessible.231 In addition to the physical
entrapment of metallic nanoparticles within the OMC scaffold,
chemical interactions can also improve the catalytic activity of
OMC supported Pt.232 Functionalizing OMC with oxygen groups
can assist in anchoring the Pt catalyst while preserving the
originally ordered structure.233 For the electrochemical oxidation
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Materials Chemistry Frontiers
of CO, this reduces the overpotential by about 100–150 mV.
Although the fundamental mechanism for this improvement has
not been elaborated yet, similar values for various OMCs have
been reported by different authors.233,234
Quite interestingly, the catalytic activity of OMC-supported
Pt depends on the OMC architecture rather than the mesopore
size.235 Fig. 12 compares the structure and electrocatalytic
activities of two OMCs having an inverse structure; while one
is an excellent catalyst support, the other is quite poor.
Pt/OMC nanocomposites show excellent electrocatalytic
behavior, e.g. for fuel cells.236–238 The electrocatalytic activity
of the Pt catalyst supported by OMC for oxygen reduction is two
times higher than that supported by commercial conductive
carbon.239 A similar behavior has been reported for the electro-
catalytic activity of Pd in alkaline fuel cells.240
It has been reported that in the preparation of OMC-
supported Pt/Ni bimetallic catalysts, the amount of Ni controls
the surface hydroxyl groups, which causes the hydrophilicity of
the OMC catalyst support.241 This significantly enhances the
electrocatalytic activity for the oxidation of methanol by facilitat-
ing the formation of Pt–OH. Another important phenomenon is
that increasing the Ni content reduces the size of bimetallic
nanoparticles, which can become smaller than the size of
mesopores. This is accompanied by a better distribution of Pt
and higher accessibility. This enhanced electrocatalytic activity
of the bimetallic catalyst is not limited to Ni. PtFex, for example,
displays exactly the same behavior.242 A vital necessity for
optimum electrocatalytic activity is the integrity of bimetallic
nanoparticles over the OMC matrix. The shape and size of the
nanoparticles should match those of the mesopores.
OMC is a good compositing agent for metal oxides, which
are promising candidates for ORR electrocatalysis, due to the
interaction of oxygen groups.243,244
Nitrogen doping improves the properties of OMC as a
catalyst support due to the presence of nitrogen coordinated
metal centers.141 This can facilitate platinum-free electro-
catalysts.245 As explained for the case of supercapacitors,
bi-dopants can further contribute to the chemical inhomogeneity
of OMC resulting in better charge transfer in electrocatalytic
reactions.246 The electrocatalytic activity of nitrogen and sulfur
co-doped OMC is comparable to that of Pt/C for the ORR.247
Doping of OMC with N and a metal can lead to superior electro-
catalysts. N and Fe co-doped OMC shows a superior electro-
catalytic activity for the ORR, even stronger than that of Pt.248
However, the influence of doping is not straightforward as
several factors are changed simultaneously. Fig. 13 shows the
effect of N-doping on Pt/OMC and Pt–Co/OMC electrocatalysts.
In contrast to the enhanced capacitive behavior of N-doped
OMC described before, N doping of Pt/OMC reduces both
capacitance and electrocatalytic activity. However, N-doping
strongly improves both the capacitive and electrocatalytic activity
of Pt–Co/OMC. This can be ascribed to several factors. The
presence of Co can enhance the graphitization of OMC. As
discussed for the bimetallic catalysts before, the presence of Co
results in smaller nanoparticles, which are comparable to the
mesopore sizes.69 Therefore, the systems are significantly different.
 View Article Online

Materials Chemistry Frontiers Review

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Fig. 12 (a and b) Schematic model, (c–f) TEM images and (g–i) electrocatalytic activities of two OMC samples synthesized using CMK-3 and FDU-15
templates. Reproduced with permission from ref. 235. Copyright 2011, Royal Society of Chemistry.

Fig. 13 CV curves of Pt/OMC, Pt/N-OMC, Pt/Co-OMC, and Pt/Co-N-OMC samples in 0.5 M H2SO4 (a) and 2.0 M CH3OH/1.0 M H2SO4 (b) with a scan
rate of 20 mV s 1. Reproduced with permission from ref. 69. Copyright 2013, American Chemical Society.

This difference is more visible for direct electrochemical oxidation
at the electrocatalysts (Fig. 13b). N doping strongly improves the
electrocatalytic activity of Pt–Co/OMC but at the price of higher
overpotentials, due to the electrochemical redox systems of N-rich
functional groups.
The electrocatalytic capability of OMC is not limited
to the catalyst support, as it can be directly used as a
metal-free catalyst.249 For this purpose, it is necessary to alter
the lattice and the surface structure of OMC by doping and
surface functionalization. Doping of OMC with various elements
such as boron,250 sulfur,251 etc. showed an acceptable electro-
catalytic activity for the ORR. Similar to the case of super-
capacitors, co-doping can further improve the electrocatalytic
activity of OMC.252

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Although OMC is chemically stable in various media including
the alkaline electrolyte, there is a gradual decrease in catalytic
activity. In the case of pure OMC, the capacitive behavior is
weakened while pseudocapacitive behavior is strengthened,
because of the formation of reactive defects and functional
groups. For doped OMCs in which there are active redox sites,
aging causes a decrease in chemical reactivity.253
The ordered mesoporous structure of OMC provides an
excellent opportunity for the formation of 1D catalysts within
the OMC structure. This feature has been utilized for in situ
synthesis of various catalysts supported on OMC.254,255
Since the pores are usually long along the OMC structure,
diffusion of electroactive species is normally unidirectional.
Modifying OMC by carbon nanotubes can create shortcuts for
charge transfer perpendicular to the pores, and thus, signifi-
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cantly improve the electrocatalytic activity.120,182 Since the
electrocatalytic activity is not controlled by the amount of
carbon nanotubes, carbon nanotubes are not real channels
for diffusion, but shortcuts opening gates in other directions
(for charge transfer rather than ion diffusion).256 The same
behavior has been reported for the OMC/CNT architecture as an
ultracapacitor.257 This is similar to the phenomenon reported
for electrodeposition in the presence of carbon nanotubes in
which the presence of carbon nanotubes within the diffusion
layer just changes the electrodeposition pathway without physical
entrapment in the depositing film.258,259 Although the silica/
carbon nanocomposite was originally an intermediary template,
it can be prepared as a free-standing film with excellent casting
capability for practical applications.260
4.7. Electrochemical hydrogen storage
Hydrogen is ideally the greenest fuel, but its applications
have been limited by difficulties in storage. In the past two
decades, carbon was a promising candidate for storing hydro-
gen in lieu of metal hydrides storing hydrogen in the bulk.
Thus, the surface structure of carbon is of particular impor-
tance for achieving an acceptable hydrogen storage capacity.
A key problem in hydrogen storage on the carbon surface is
that adsorbed H atoms can interact with each other to form
H2 and leave the material in gaseous form. OMC seems to
be a promising candidate, as adsorbed atoms are somehow
entrapped within the mesopores. In addition to the morpho-
logical structure, chemical functionality also plays a substantial
role in the hydrogen storage capacity of OMC. It has been
reported that while oxidized nitrogen functional groups may prevent
the adsorption of hydrogen, N-doped OMC showed 1.5 times
enhancement in electrochemical hydrogen storage.261,262
While OMC stores hydrogen by surface interaction, metals
can store hydrogen in the form of metal hydride. Mixing metal
nanoparticles with OMC can assist catalytic hydrogen to dis-
sociate for absorption on the carbon surface while contributing
to the hydrogen storage in the form of metal hydride. The
Ni/OMC nanocomposite showed a good capacity for electro-
chemical hydrogen storage.263 As mentioned above, Ni can
improve the hydrophilicity of OMC due to the hydrogen func-
tional groups. The capability of OMC-supported Pt/Ni for
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Materials Chemistry Frontiers
electrochemical hydrogen storage is increased three times when
the Ni content is increased from 2 to 15%.241 A similar behavior
has also been observed for OMC-supported NiFe too.264
There is great flexibility for doping of OMC targeting electro-
chemical applications. Cu and N were utilized as dopants to
improve the capacity of OMC for electrochemical hydrogen
storage.265
5. Summary and outlook
OMC has attracted considerable attention during the past
5 years for potential applications in various electrochemical
energy storage and conversion systems. However, OMC is somewhat
considered as a standard material with well-defined architecture,
which may be misleading. In practice, at least in electrochemical
systems, OMCs are very complicated materials which represent
some kind of order at the mesoscale. Both the chemical structures
of the pore walls and edges are critically important in electro-
chemical systems, but less attention is usually paid to comparing
similar OMCs in a specific application. On the other hand, not
only is the interconnection of the mesopores of essential impor-
tance, but also the packing of the material particles can define
the overall accessibility of the mesopores. In other words, in a
compact electrode, the OMC architecture is not as ordered as
seen in the TEM images.
Along with the increasing interest in OMC, there have
appeared reports in the literature claiming the unsuitability
of OMC for many electrochemical systems. Here, we attempted
to highlight two aspects of this potential material: (i) it is a fact
that OMC is not as charming and ideal as it is seen in TEM
images, and (ii) possible weak performance in electrochemical
systems is not necessarily the incapability of OMC for conducting
the electrochemical reaction within its ordered architecture. In
general, OMC should be specifically tuned for various applica-
tions including those of electrochemical energy storage and
conversion systems. Some of the reports available in the literature
clearly show the potential of OMC for various electrochemical
systems, but the ‘‘one size fits all’’ strategy does not work here.
The main obstacle for the practical application of OMC in
electrochemical energy systems is the lack of an appropriate
synthesis route for the mass production of OMC while design-
ing its architecture for the electrochemical cell. While the
conventional silica template method is ideal for the prepara-
tion of highly ordered mesopores at a lab scale, there is still no
practical approach for scaling up this synthesis route. On the
other hand, soft-template methods or other hard templates are
more practical for mass production, but at the cost of losing the
highly ordered architecture of OMC to some extent. Combining
these methods might be a subtle approach for the practical
production of OMC. Owing to the essential importance of the
pore directions in the OMC architecture, not only the synthesis
but also the arrangement of the OMC particles in the electrode
composite is of practical importance. Therefore, the OMC
should be prepared as a film or directly grown on the current
collector to guarantee the original electrochemical properties.

Materials Chemistry Frontiers
In conclusion, we need more fundamental studies to under-
stand how the OMC atomic structure controls the electro-
chemical processes, instead of typical examinations of OMCs 13
in different systems.
Acknowledgements 14
Z. F. acknowledges the support from the National Science
Foundation (1611060).
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