Bi2WO6/PANI: An efficient visible-light-induced photocatalytic composite

Article abstract of DOI:10.1016/j.cattod.2013.11.030

Bi₂WO₆ photocatalyst film prepared by a facile chemical bath deposition (CBD) method was modified by polyaniline (PANI) through in situ polymerization of vapor phase aniline. The photocatalytic activities of the PANI/Bi₂WO₆ film were evaluated by the degradation of a widely used dye, tetraethylated rhodamine (RhB), and a general gaseous indoor air pollutant, acetaldehyde under visible-light irradiation (λ > 420 nm). The excellent performance of the PANI/Bi₂WO₆ film could be attributed to the rapid separation and slow recombination of the photogenerated electron-hole pairs contributed by the synergic effect between PANI and Bi₂WO₆. The stability of the photocatalytic film is found to be satisfying, which makes it potential in practical application. This work not only solves the separation and recycling problem for nano-sized photocatalyst, but also provides insight into the design of photocatalytic film with high activity for environmental applications, especially for indoor air purification.

Full text of DOI:10.1016/j.cattod.2013.11.030

Catalysis Today 224 (2014) 147–153
Contents lists available at ScienceDirect
Catalysis Today
journal homepage: www.elsevier.com/locate/cattod
Bi2WO6/PANI: An efficient visible-light-induced photocatalytic
composite
Wenzhong Wang∗, Jiehui Xu, Ling Zhang, Songmei Sun
State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences,
1295 Dingxi Road, Shanghai 200050, PR China
a r t i c l e i n f o
a b s t r a c t
Article history:
Received 31 July 2013
Received in revised form 23 October 2013
Accepted 1 November 2013
Available online 9 December 2013
Bi2WO6 photocatalyst film prepared by a facile chemical bath deposition (CBD) method was modified by
polyaniline (PANI) through in situ polymerization of vapor phase aniline. The photocatalytic activities
of the PANI/Bi2WO6 film were evaluated by the degradation of a widely used dye, tetraethylated rho-
damine (RhB), and a general gaseous indoor air pollutant, acetaldehyde under visible-light irradiation
(ꢀ > 420 nm). The excellent performance of the PANI/Bi2WO6 film could be attributed to the rapid sep-
aration and slow recombination of the photogenerated electron–hole pairs contributed by the synergic
effect between PANI and Bi2WO6. The stability of the photocatalytic film is found to be satisfying, which
makes it potential in practical application. This work not only solves the separation and recycling prob-
lem for nano-sized photocatalyst, but also provides insight into the design of photocatalytic film with
high activity for environmental applications, especially for indoor air purification.
Keywords:
Bi2WO6
Polyaniline
Photocatalytic film
Visible light
© 2013 Elsevier B.V. All rights reserved.
1. Introduction
Bi2WO6 film possesses notable advantages in the decomposition
of gaseous contamination especially in static system. The inter-
Photocatalysis is considered as a promising technique for the
purification of polluted water and air. With the increasing demand
of directly utilizing solar energy, the development of visible light
responsive photocatalyst is becoming one of the goals in the
research of photofunctional materials. Bi2WO6, with a band gap
of 2.6–2.8 eV, has exhibited relatively high efficiency in the visible
light induced photocatalyst for mineralizing organic contaminants
(apparent quantum efficiency under 400 nm irradiation, ∼8%) with-
out any surface modification [1]. Recently, it has been extensively
investigated as a potential visible light induced photocatalyst [2–5].
However, few studies were focused on the preparation of films
which is beneficial for practical photocatalytic application. And the
film deposition methods mainly fasten on the dip-coating method
for its easy processing [6–9]. To achieve better adherence to the
substrate, for the first time, we deposited Bi2WO6 photocatalyst
with well-defined morphology on stainless steel mesh through a
chemical bath deposition (CBD) method.
face between the photocatalyst and contaminant was increased
because the Bi2WO6 particles were well dispersed on the substrate
with high surface area, rather than agglomerated together in the
static degradation system of photocatalyst powders. To improve
the photocatalytic activity further, promotion of the separation
efficiency of photogenerated electron–hole pairs is considered to
be one of the most effective ways [10]. Coupling with materials
of delocalized conjugated structures is such an efficient approach,
because rapid photoinduced charge separation and relatively slow
charge recombination in electron-transfer processes were realized
[11]. In particular, polyaniline (PANI), as one of the most impor-
tant intrinsically conducting polymers (ICPs) with an extended
ꢁ-conjugated electron system, has recently showed great promises
due to its high absorption coefficients in the visible-light range
and high mobility of charge carriers [12]. Taking account of the
efficient carrier-transfer property of PANI, it is expected that the
coupling of photocatalyst and PANI would be ideal for enhanc-
ing the activity under visible light. As reported, however, most of
photocatalysts were coupled with PANI through a simple dipping
procedure [13–15]. Although it is convenient since no further treat-
ment was involved, the adherence between PANI and substrate
through physical adsorption is not firm enough. Several groups
reported the deposition of ICP layers by in situ polymerization tech-
niques, where the substrate materials were successively coated by
oxidant and monomer layers, in solution or vapor phase [16–20].
This flexible method essentially allows the addition of electronic
For photocatalytic films, the significant loss of active sites on
the surface of the photocatalyst limits its efficiency in the photo-
catalytic degradation of pollutants. Our previous work has reported
a way to improve it by developing new kind of reticular stainless
steel mesh substrate with large surface area [9]. The as-prepared
∗
Corresponding author. Tel.: +86 21 5241 5295; fax: +86 21 5241 3122.
E-mail address: wzwang@mail.sic.ac.cn (W. Wang).
0920-5861/$ – see front matter © 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.cattod.2013.11.030

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W. Wang et al. / Catalysis Today 224 (2014) 147–153
Scheme 1. The process of in situ polymerization of PANI on Bi2WO6 film by CBD method.
properties to film (with optimized mechanical properties) using
standard coating procedures.
2.2. Characterization of PANI/Bi2WO6 photocatalytic film
In this study, the Bi2WO6 photocatalyst film prepared by CBD
method was modified with PANI by vapor-phase techniques. The
PANI coating process was realized by an in situ polymerization
instead of dipping procedure. The photocatalytic activity and sta-
bility of as-prepared PANI/Bi2WO6 film were evaluated by the
degradation of contaminants in aqueous/gaseous phases under vis-
ible irradiation (ꢀ > 420 nm). Moreover, we aimed to approach the
possible mechanism of the improved activity in order to guide fur-
ther work for the improvement of photocatalytic performance.
The purity and crystallinity of the as-prepared Bi2WO6 powders
and films were characterized by powder X-ray diffraction (XRD)
with a Rigaku D/MAX 2250 V diffractometer using monochroma-
tized Cu K␣ (ꢀ = 0.15418 nm) radiation under 40 kV and 100 mA and
scanning over the range of 20◦ ≤ 2ꢂ ≤ 70◦. The morphologies and
microstructures characterizations were performed on the scan-
ning electron microscope (SEM, JEOL JSM-6700F). UV–vis diffuse
reflectance spectra (DRS) of the samples were obtained on an
UV–vis spectrophotometer (Hitachi U-3010) using BaSO4 as the
reference.
Photocatalytic activities of the samples were evaluated by
the degradation of model contaminants under the irradiation of
a 500 W Xe lamp with a 420 nm cutoff filter. For the decol-
orization of RhB, 0.1 g of Bi2WO6 photocatalyst was added into
100 mL of RhB solution (10−5 mol/L) and stirred in the dark
for 2 h before illumination to ensure the establishment of an
adsorption–desorption equilibrium between the photocatalyst and
RhB. For the Bi2WO6 film samples, they were placed into 50 mL of
RhB solution (10−5 mol/L) and kept in the dark for 2 h to ensure
the adsorption–desorption equilibrium. At 10 min or 30 min inter-
vals, the absorption of a 3 mL of sample solution was recorded on
a Hitachi U-3010 UV–vis spectrophotometer. For the degradation
of acetaldehyde (CH3CHO), the film was placed at the bottom of
a gas-closed reactor with a quartz window at room temperature
(capacity 600 mL). The reaction gas mixture (1 atm) consisted of
100 ppm CH3CHO and N2 balance gas. Prior to irradiation, the reac-
tion system was equilibrated for about 30 min until no change in
the concentration of CO2 was monitored. Gaseous samples (1 mL)
were periodically extracted and analyzed by a gas chromatograph
(GC) equipped with a flame ionization detector (N2 carrier) and a
catalytic conversion furnace.
2. Experimental
2.1. Preparation of PANI/Bi2WO6 film
All the chemicals were analytical grade reagents from Shanghai
Chemical Company and used without further purification. Bi2WO6
film has been deposited on the substrate of twill weaved 400
meshes stainless steel mesh made of SUS 304 (5 × 5 cm). Before
deposition, the substrates were cleaned by sonication for 15 min
in anhydrous ethanol and dilute hydrochloric acid (1 wt.%) respec-
tively and then rinsed with deionized water. In a typical procedure,
Bi(NO3)3•5H2O and Na2WO4•2H2O, in a molar ratio of 2:1, were
dissolved in the mixed solvent of ethylene glycol (EG) and
2-methoxyethanol (2-MOE), in a volume ration of 1:3. The con-
centrations of Bi2WO6 in the bulk solution ranged from 5 to
12.5 mmol/L (mM). The pre-treated substrates were immersed in
the above solution for about 1 h to facilitate nucleation on the sub-
strate surface [21], and then the solution was refluxed at 120 ◦C for
12 h. Afterwards, the film and particles in the solution were col-
lected, rinsed with anhydrous ethanol and deionized water, and
then oven-dried at 60 ◦C. For better crystallization, the obtained
film and particle samples were thermal treated at 450 ◦C for 1 h in
air.
3. Results and discussion
The PANI coating process is described in Scheme 1. The annealed
CBD films were dipped into an ammonium persulfate (APS) solu-
tion. 2% (v/v) of concentrated HCl was added to the oxidant solution
in order to obtain the acid doping PANI coating layer which is con-
ductive. Excess APS solution was wiped off. The films were then
transferred into a reactor which was heated by hot plate at 40 ◦C to
make the monomer solution of aniline evaporate. The monomer
vapors polymerized when they came in contact with the APS-
coated films, producing a thin PANI coating, doped with H+ ions. The
polymerization time was set as 1 h. Afterwards, the obtained film
was collected and rinsed with anhydrous ethanol and deionized
water and then oven-dried at 60 ◦C.
As a one-step, low-energy-consumption technique, chemical
bath deposition (CBD) has been widely applied for depositing
large-area films with particular shape, orientation and thick-
ness [22,23], in which thin films are deposited on the substrates
immersed in dilute solutions. This process is on the base of the
controlled precipitation of the metal ion in the reaction bath.
Many metal chalcogenide (including sulfides, selenides) and simple
metal oxides thin films have been prepared by CBD [24–26]. How-
ever, multiple metal oxide functional films were rarely deposited
through this process. This could be ascribed to the critical phase for-
mation temperature of the multiple metal oxides which is mainly

W. Wang et al. / Catalysis Today 224 (2014) 147–153
149
well with those of the monoclinic phased Bi2O3 according to the
JCPDS 65-2366, accompanied by the diffraction of the stainless
steel substrate. In contrast, the film deposited at higher concen-
tration of 10 mM matched well with orthorhombic Bi2WO6, again,
except for the peaks of substrate. The diffraction profiles reveal
that Bi2WO6 are well crystallized after calcination and the broad
diffraction peaks imply that the crystalline grains are on nanoscale.
To further investigate the influence of concentration on the mor-
phological evolution process of the Bi2WO6 film, a series of SEM
images of calcined films obtained at different concentrations were
revealed in Fig. 2. As it has been verified that Bi2WO6 phase can only
be obtained at higher concentration, the particles differed in size
and shape. At lower concentration, Bi2O3 particles were obtained
and they were smaller and closely packed into larger agglomerates.
They tended to aggregate on bent parts of stainless steel wire with
high surface energy instead of uniformly coat on the whole part of
the wire (Fig. 2a–d). While at higher concentration, the size distri-
bution of Bi2WO6 particles was uniform consisting of spheres with
a diameter of 400–500 nm. Higher concentration favored to form
larger particles and thicker coating layers (Fig. 2g and h). As no sur-
factants were involved, these nanoparticles were quickly built and
spontaneously aggregated to minimize their surface area through
the process known as Ostwald ripening.
Photocatalytic degradation of RhB was performed under visible
light irradiation (ꢀ > 420 nm) to evaluate the photocatalytic proper-
ties of the Bi2WO6 powders and films. RhB, a representative textile
dye, showed a major absorption band at 553 nm. Fig. 3 displays the
temporal evolution of the spectral changes during the photodegra-
dation of RhB by Bi2WO6 powders (a) and film (b) obtained at the
concentration of 10 mM Bi2WO6 in the bulk solution. A decrease of
RhB absorption at a wavelength of 553 nm was observed, along with
absorption band shifts to shorter wavelengths. The destruction
of the dye chromophore structure was induced by the predom-
inant oxidation of the hydroxyl radicals (photogenerated holes)
localized at the surface of irradiated photocatalyst [28]. Compared
to the slurry system, the photocatalytic activity of Bi2WO6 film
decreased dramatically. Nearly 100% of RhB was decolorized by the
Bi2WO6 powders under visible light in 30 min, however, only 59%
by Bi2WO6 film under the same condition. It took more than 3 h to
decolorize 100% of RhB by the film. The immobilization of the pho-
tocatalyst led to significant reduction of the interface between the
photocatalyst and contaminant, which remains the major obstacle
in the application and popularization of photocatalysis technology.
For the significant loss in the activity in the photocatalytic degra-
dation of pollutants because of the decrease of active sites on the
surface of the photocatalyst, PANI was coupled to promote the sepa-
ration efficiency of photogenerated electron–hole pairs. The in situ
vapor-phase polymerization method was introduced on the sur-
face of Bi2WO6 film. The polymerization of aniline was observed as
the appearance of the film changed from yellowish to green. The
diffuse-reflection spectra (DRS) of the Bi2WO6 and PANI/Bi2WO6
films are depicted in Fig. 4. The Bi2WO6 film sample exhibited
photoabsorption from UV light to visible light, and the absorp-
tion edge locates at 450 nm. The absorption of the PANI/Bi2WO6
film sample increases over nearly the whole range of the spec-
trum. Therefore, the PANI-modified Bi2WO6 film can be excited
to produce more electron–hole pairs under the same visible-light
illumination, which could result in higher photocatalytic activity.
The photodegradation efficiency of RhB by PANI/Bi2WO6 film
which is displayed in Fig. 5 verified the synergetic effect of PANI
on the photocatalytic activity of Bi2WO6. As shown, the adsorp-
tion of RhB on the PANI/Bi2WO6 film is stronger than that on the
Bi2WO6 film after 2 h in the dark. The concentration of RhB decrease
obviously under the irradiation of visible light within 1.5 h, suggest-
ing the decolorizing of RhB was photodegraded by PANI/Bi2WO6
film. Comparison of the photodegradation efficiency with pure
Fig. 1. XRD patterns of the Bi2WO6 powders by CBD process at different concentra-
tions (a) and the calcinated films at the concentration of 5 and 10 mM (b).
higher than those of the metal chalcogenide. Moreover, sponta-
neous precipitation of Bi2WO6 occurs when aqueous solutions
containing salts of Bi3+ and WO4
are mixed which will lead to
2−
the formation of large particles. This procedure yields particles
without morphology control resulting in bad adherence to the sub-
strates, which favors the formation of dispersed particles rather
than being deposited on the substrates. In order to prepare Bi2WO6
particles with well-defined morphology, the reaction conditions
should be well controlled so as to the nucleation and growth of the
solid [27]. Herein, the mixed solvent of ethylene glycol (EG) and 2-
methoxyethanol (2-MOE) was utilized to prevent the hydrolysis of
Bi3+ and avoid the spontaneous precipitation of Bi3+ and WO42−, via
the unique coordination of EG and 2-MOE. Compared to pure sol-
vent of EG, the mixed solvent containing 2-MOE not only decrease
the refluxing temperature because of its low boiling point, but also
maintain the coordination with Bi3+ and WO4
.
2−
The influence of initial concentration of the precursor (5, 7.5, 10,
and 12.5 mM) on the formation of Bi2WO6 phase was checked. The
phase and composition of the Bi2WO6 particles collected after the
deposition process were given in Fig. 1a. At lower concentrations
(5 and 7.5 mM), the peaks were weak with noisy background while
they were identified as some intermediate products such as ammo-
nium tungstate. While at higher concentration (10 and 12.5 mM),
although the product was poorly crystallized, the XRD pattern can
be indexed to orthorhombic Bi2WO6 (JCPDS 39-0256). The calcina-
tion process favors the formation of good crystallization, and the
diffraction peaks of calcined films were demonstrated in Fig. 1b. As
shown, at the concentration of 5 mM, the diffraction peaks agree

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W. Wang et al. / Catalysis Today 224 (2014) 147–153
Fig. 2. SEM images of as-synthesized Bi2WO6 films by CBD process at different concentrations (from 5 mM to 12.5 mM) of low (a, c, e, g) and high (b, d, f, h) magnifications.
Bi2WO6 film is revealed in Fig. 5b, where C is the concentration
of RhB at the irradiation time t and the C0 is the initial con-
centration when the adsorption–desorption equilibrium between
photocatalyst and RhB was established in dark. It was displayed
that less than 80% RhB can be degraded by pure Bi2WO6 film under
visible light in 1.5 h. Therefore, the PANI/Bi2WO6 film exhibited
higher photodegradation efficiency with higher absorption capa-
bility compared with pure Bi2WO6 film.
Besides the enhanced photocatalytic activity resulting from
PANI, the photostability of the photocatalyst was also retained [14].
The circulating runs in the photocatalytic degradation of RhB in
the presence of PANI/Bi2WO6 film under visible light (ꢀ > 420 nm)

W. Wang et al. / Catalysis Today 224 (2014) 147–153
151
Fig. 3. RhB aqueous solution (10−5 mol/L) degradation in the presence of the Bi2WO6
powders (a) and film (b) by CBD process at the concentration of 10 mM under visible-
light irradiation (ꢀ > 420 nm).
Fig. 5. RhB aqueous solution (10−5 mol/L) degradation in the presence of the
PANI/Bi2WO6 film (a) and the changes of temporal UV–vis spectral of RhB by Bi2WO6
and PANI/Bi2WO6 film under visible-light irradiation (ꢀ > 420 nm).
were checked. Fig. 6 shows C/C0 as a function of time, where C is
the concentration of RhB at the irradiation time t and the C0 is the
initial concentration when the adsorption–desorption equilibrium
between photocatalyst and RhB was established in dark. After five
cycles for the photodegradation of RhB, the activity of the photo-
catalyst did not exhibit any significant loss. It indicates that the
PANI/Bi2WO6 photocatalytic film has high stability and does not
photocorrode during the photocatalytic oxidation of the model pol-
lutant molecules. PANI is also cheaper than noble metals; thus, the
PANI/Bi2WO6 photocatalytic film is promising for practical appli-
cation in water purification.
To further confirm the photocatalytic properties of the as-
prepared PANI/Bi2WO6 film and eliminate the photosensitive
effect of RhB, gaseous acetaldehyde (CH3CHO) was selected to
evaluate the photocatalytic activity. Different from RhB, CH3CHO
Fig. 4. UV–vis diffuse reflectance spectra of the as-synthesized Bi2WO6 and
PANI/Bi2WO6 film.
Fig. 6. Cycling experiment of the photocatalytic degradation of RhB in the presence
of PANI/Bi2WO6 film under visible-light irradiation (ꢀ > 420 nm).

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W. Wang et al. / Catalysis Today 224 (2014) 147–153
Scheme 2. Schematic diagram for energy band matching and migration and sepa-
ration of electron–hole pairs in the coupled PANI/Bi2WO6 system.
Fig. 7. Photocatalytic activity of PANI/Bi2WO6 film for the degradation of acetalde-
hyde (100 ppm) in air under visible light (ꢀ > 420 nm).
does not absorb light; thus, the photosensitization process does
not exist in such a photodegradation process. As shown in Fig. 7,
CH3CHO was degraded by the Bi2WO6 and PANI/Bi2WO6 film with
an obvious production of CO2 under visible light irradiation. The
PANI/Bi2WO6 film exhibited higher activity in the degradation of
CH3CHO than pure Bi2WO6 film. For comparison, the photodegra-
dation of CH3CHO by 0.05 g Bi2WO6 powders which were collected
during CBD process was also tested. In gaseous system, the powders
showed a comparatively low photocatalytic activity. After being
irradiated for 3 h, CH3CHO was degraded almost completely by
the PANI/Bi2WO6 film with the production of about 200 ppm CO2,
and nearly 80% of CH3CHO was degraded by pure Bi2WO6 film.
However, the decomposition of CH3CHO by Bi2WO6 powders was
less than 50% after the same irradiation time. The enhanced pho-
tocatalytic activity of the film compared with powders could be
attributed to the new type of substrate. It increased the interface
between the photocatalyst and contaminant because the photo-
catalyst particles were well dispersed on the substrate with high
surface area, rather than agglomerated together in the static degra-
dation system of catalyst powders. As a blank experiment, the
PANI/Bi2WO6 film sample was irradiated under the same experi-
mental condition without CH3CHO in the reactor. No production
of CO2 was detected, which indicated no photolysis of CH3CHO
exists. Therefore, the degradation of CH3CHO was fully attributed to
the photocatalytic process. Furthermore, the PANI/Bi2WO6 film did
not produce any CO2 itself under visible light irradiation, verifying
stability of the PANI/Bi2WO6 film once again.
in charge separation and stabilization, thus hindering the recom-
bination process. PANI is a good material for transporting holes,
and the grain size of the photocatalyst is also relatively small [31];
therefore, the photogenerated charges can emigrate to the surface
of photocatalysts and photodegrade the adsorbed contaminations.
With the synergic effect, the photocatalytic ability of PANI/Bi2WO6
film is improved remarkably. Further efforts are mainly focused
on optimizing the content of coating PANI to improve the pho-
tocatalytic activity of PANI/Bi2WO6 film for practical application.
Although the photocatalytic efficiency of the film is not compara-
ble to that of the Bi2WO6 powders, the cost which is saved during
the separation and recycling process makes this film promising
for future environmental application, especially in the indoor air
purification.
4. Conclusion
In conclusion, a CBD method was developed to deposit the
Bi2WO6 photocatalyst on the reticular substrate of stainless steel
mesh. The method involves mild temperatures and yields morpho-
logical well-defined Bi2WO6 nanoparticles. This coating process
may be extended to the deposition of Bi2WO6 on various types
of substrate and technological coating of other relevant photocata-
lysts. Compared to the slurry system, the photocatalytic activity of
the as-prepared Bi2WO6 film decreased dramatically after immo-
bilization, because of significant reduction of the interface between
the photocatalyst and contaminant.
The photocatalytic activity of Bi2WO6 film was enhanced by the
modification of PANI with intrinsic properties. The synergic effect
between PANI and Bi2WO6 was realized through an in situ poly-
merization of aniline. The PANI/Bi2WO6 film exhibited efficient
photocatalytic activity and excellent stability in oxidative decom-
position of RhB under visible light (ꢀ > 420 nm). In particular, the
degradation of gaseous acetaldehyde eliminated the photosensi-
tive effect of RhB, and verified the stability of the PANI/Bi2WO6
film once again. The excellent properties of the PANI/Bi2WO6 film
were mainly ascribed to the rapid separation and slow recombina-
tion of the photogenerated electron–hole pairs. From the viewpoint
of practical application, this work does not only solve the separa-
tion problem which is general for photocatalyst particles in slurry
system, but also provided some insight into the design of photo-
catalysis film with high activity for environmental applications,
especially the indoor air purification.
The above experiments have shown the excellent photocatalytic
performance of the as-prepared PANI/Bi2WO6 on the degradation
of the widely used dye and common indoor air pollutant. It follows
that the PANI modified Bi2WO6 photocatalysis film may have highly
potential applications in the conservation of the environment.
Not only limited to the experimental results, the photodegraded
mechanism of contaminants under visible light was necessary to
investigate and guide the further improvement of its photocatalytic
performance. The possible photocatalytic mechanism (Scheme 2)
was proposed as follows:
Bi2WO6
PANI
hꢃ
−→ h+ + e−
(1)
On the basis of the relative energy level of PANI (ꢁ-orbital
and ꢁ*-orbital) and Bi2WO6 (conduction band, CB, and valence
band, VB) [29,30], the photogenerated holes in VB can directly
transfer to the ꢁ-orbital of PANI. Simultaneously, the photogen-
erated electrons can transfer to the CB of Bi2WO6, which results

W. Wang et al. / Catalysis Today 224 (2014) 147–153
153
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