Industrial Crops & Products xxx (xxxx) xxx

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Industrial Crops & Products

journal homepage: www.elsevier.com/locate/indcrop

Utilization of bark waste of Acacia mangium: The preparation of activated

carbon and adsorption of phenolic wastewater
Feihu Zhang , Sheng Zhang *, Lei Chen , Zilei Liu , Junjie Qin
College of Materials Science and Engineering, Central South University of Forestry and Technology, Changsha, Hunan, 410004, China

A R T I C L E I N F O A B S T R A C T

Keywords: After the extraction of industrial tannins from Acacia mangium, there is a lot of bark waste. Thus, we use these
Bark waste of Acacia mangium bark wastes to produce activated carbon using the phosphoric acid activation method. The information entropy
Activated carbon weight method is employed to select the best process according to the weight coefficients of the activated carbon
Phenol adsorption
yield and value of methylene blue adsorption. In this study, the phenol adsorption behaviors of activated carbon
and its thermodynamic and kinetic characteristics are investigated. The results indicate that the best process for
the preparation of activated carbon from the bark waste of Acacia mangium involves phosphoric acid concen­
tration of 50 %, carbonization temperature of 500◦ C, and carbonization time of 90 min. Under these conditions,
activated carbon obtained from the bark waste of Acacia mangium in this study is 53.04 %, and the value of
methylene blue adsorption is 6.0 mL/0.1 g. In liquid, the adsorption capacity of activated carbon increases with
the initial content of phenol, and the highest value is around 96.92 mg g− 1, which is obtained at 25◦ C. The
adsorption thermodynamic is well expressed by the Freundlich isotherm adsorption equation, and the adsorption
behavior curves flow McKay second-order adsorption kinetic equation. This result indicates that phenol waste­
water is absorbed very well by activated carbon prepared from the bark waste of Acacia mangium. This study lays
the foundation for further development of biomass-activated carbon strategy and provides a promising insight
into the enhancement utilization of Acacia mangium.

1. Introduction tannins, which are complex phenolic substances (Seigler, 2003).

As an industrial crop, Acacia mangium is a large evergreen tree that
belongs to the genus Acacia of the Mimosa subfamily. It is mainly
distributed in India, Southeast Asia, and the southern provinces of China
(Zhang et al., 2010a, 2010b). This tree is considered to be a nurse plant
for understory plants (Yang et al., 2009). It has been reported that the
content of condensed tannins in the bark of Acacia mangium is as high as
40 %, which is used for the extraction of tannins (Hoong et al., 2009;
Bharudin et al., 2013).
Tannins from Acacia mangium exhibit good stability, low viscosity,
fast permeability, and strong adsorption. They can be used to prepare
bio-based adhesives (Hoong et al., 2009, 2010, 2011).
Numerous secondary metabolites have been discovered in the bark of
Acacia mangium that contains amines and alkaloids, cyanogenic glyco­
sides, cyclitols, fatty acids and seed oils, gums, nonprotein amino acids,
terpenes (including essential oils, diterpenes, phytosterol, triterpene
genins, and saponins), hydrolyzable tannins, flavonoids, and condensed
tannins. Among them, the most widely used and studied are condensed
Although the annual discharge of BWA (bark waste of Acacia man­
gium) from a medium-sized tannin extract plant is nearly 1.000 × 106 kg,
the utilization of bark waste is limited and mostly used as fuel (Taflick
et al., 2017), fertilizer (Silva et al., 2020), and culture medium for edible
mushroom (Rizki and Tamai, 2011).
In the chemical industry, phenol is an important raw material for
organic chemical products. It can be used to produce caprolactam,
bisphenol A, phenol resin, pentachlorophenol, salicylic acid, phenol­
phthalein n-acetylethoxyaniline, and other chemical products (Singh
et al., 2009; Kang et al., 2015; Luo et al., 2018). During the chemical
production process, a large amount of phenolic wastewater is discharged
(Zhang et al., 2010a, 2010b; Ahmadreza et al., 2019). As a carcinogen,
phenol is highly toxic and corrosive, and can cause severe harmful
consequences on both human and ecosystem (Wierzba et al., 2017;
Yasar Arafath et al., 2019; Wang et al., 2019). Therefore, the effective
control of phenolic wastewater is an urgent problem that needs to be
solved. Currently, the main methods for the treatment of
phenol-containing wastewater include membrane separation (Raza

* Corresponding author.
E-mail address: gingshen123@126.com (S. Zhang).

https://doi.org/10.1016/j.indcrop.2020.113157
Received 30 April 2020; Received in revised form 15 November 2020; Accepted 24 November 2020
0926-6690/© 2020 Elsevier B.V. All rights reserved.

Please cite this article as: Feihu Zhang, Industrial Crops & Products, https://doi.org/10.1016/j.indcrop.2020.113157
F. Zhang et al.
et al., 2019), coagulation-precipitation (Golbaz et al., 2014), photo­
chemical oxidation (Malakootian and Heidari, 2018), electrochemical
oxidation (Liu et al., 2019), biodegradation (Ren et al., 2017), and
adsorption (El-Naas et al., 2017). Among these methods, adsorption has
been found to be more advantageous owing to its simple process,
regenerative capacity, high efficiency, and low cost (Zazycki et al.,
2018).
In the adsorption process, activated carbon is widely used owing to
its large specific surface area, developed pore structure, high adsorption
efficiency, and good chemical stability (Lu et al., 2011). Mesopores are
channels for adsorbate molecules, and capillary condensation occurs to
adsorb macromolecules (Nakagawa et al., 2004).
Thus, mesoporous activated carbon is considered to be suitable for
the liquid-phase adsorption of phenol. Activated carbon can be prepared
in two stages, namely, carbonization and activation (Okman et al.,
2014). In the carbonization process, non-carbon elements, such as
hydrogen and oxygen, in the substance become volatile gases and escape
under the conditions of high temperature and oxygen deficiency (Ali
et al., 2012). In this process, the carbonaceous material is pyrolyzed into
porous carbonized material, generating edge carbon atoms with unsat­
urated chemical bonds. It reacts with heterocyclic atoms existing on the
carbon surface, such as hydrogen, nitrogen, oxygen, phosphorus, and
sulfur, to form different surface groups. These functional groups are
combined with the adsorbed molecules through chemical bonds, which
selectively adsorb polar and nonpolar substances (Julien et al., 1998;
Cam et al., 2013). In the activation process, gases, such as H2O and CO2,
or chemical reagents, such as H3PO4, ZnCl2, K2CO3, and KOH, are used
to further process the carbonized material, change its internal structure,
and expand its specific surface area (González-García, 2018). The
biggest disadvantage of the KOH activation method is that it causes
corrosion to the equipment. During the activation process, potassium
vapor is generated, which seriously causes pollution to the environment
(Prahas et al., 2008). Therefore, this method has higher requirements for
equipment, and there is also an increase in the production cost.
Compared with the KOH activation method, the ZnCl2 activation
method requires lower activation temperature and lower requirements
for the equipment. However, ZnCl2 is volatile and can also cause serious
pollution to the environment (Shu et al., 2013). The activation tem­
perature of K2CO3 and oxidizing gases, such as CO2, H2O, and O2, is
high, and the activation time is long (Román et al., 2013). Contrarily,
the H3PO4 activation method requires a low activation temperature
(Gupta et al., 2013). In addition, the prepared activated carbon exhibits
a relatively developed pore structure and high yield. Compared with the
KOH and the ZnCl2 activation methods, the H3PO4 activation method
has the advantages of less environmental pollution and low production
cost (Jawad et al., 2017).
Although there are numerous studies on the removal of pollutants
from an aqueous solution using bark as a biosorbent or its modified
derivatives, such as activated carbon, very few have considered the use
of Acacia mangium bark, especially the BWA, for the preparation of
activated carbon. In this study, BWA was used to produce activated
carbon using the phosphoric acid method. The specific surface area and
pore-size distribution of activated carbon were determined. In addition,
the information entropy weight method was employed for the selection
of the best process according to the weight coefficients of the activated
carbon yield and value of methylene blue adsorption. The adsorption
effect of activated carbon on phenolic wastewater and its thermody­
namic and kinetic characteristics were studied. Compared with Şen
et al., 2015, organic matter instead of heavy metal ions was adsorbed by
activated carbon from bark waste of Acacia mangium after tannin
extraction in our study. Compared with Gao et al., 2016, to support
application for the activated carbon from bark waste of Acacia mangium,
both process optimization and adsorption behaviors of the activated
carbon were presented in our study. Compared with Lütke et al., 2019,
phosphoric acid activation method to prepare activated carbon in our
study is less irritating than zinc chloride activation method in the
2
Industrial Crops & Products xxx (xxxx) xxx
references. In addition, information entropy weighting method to pro­
cess data make the results more objective. Thus, this study can provide
basic knowledge on the converted process of activated carbon produced
from BWA, considering the potential possibility of application in a
comprehensive ecological improvement.
2. Material and methods
2.1. Material and reagents
BWA was obtained from Wuming Tannin Extract Factory (Guangxi,
China). The BWA was cut into pieces in the size of 3− 5 mm and then
dried at a temperature of 105◦ C for 24 h to prepare the activated carbon.
We found that the bark waste contains 23.15 % lignin, 35.41 % cellu­
lose, and 15.42 % hemicellulose.
Potassium dihydrogen phosphate, disodium hydrogen phosphate,
methylene blue, anhydrous copper sulfate, phenol, phosphoric acid (all
are of analytical grade), and methanol (HPLC grade) were obtained from
Sinopharm Chemical Reagent Co., Ltd. (Shanghai, China).
2.2. Preparation of activated carbon from BWA
In this study, a single-factor experiment was applied to explore the
preparation conditions for activated carbon using the phosphoric acid
activation method with a fixed material-to-liquid ratio of 1:2.
BWA powder was oven-dried to a constant weight at 105℃. Five
samples (1.5 g of BWA powder mixed with 30, 40, 50, 60, and 70 %
phosphoric acid solution (mass concentration) were prepared in a 50 mL
porcelain crucible.
The samples were sealed with plastic wrap and kept for 24 h, oven-
dried at 65◦ C to complete the pretreatment, and then carbonized and
activated at 500◦ C for 120 min in SX-12− 10 box resistance furnace
controller (Tianjin Taisite Instrument Co., Ltd., China). The carbonized
product was then transferred to a suction filter unit, repeatedly washed
with deionized water till it reached neutral pH, and then oven-dried to a
constant weight at 105℃. The adsorption capacity was determined
using the methylene blue adsorption value method (GB 12496.10 1999).
First, the dry activated carbon was ground and passed through a 200-
mesh sieve. Then, 0.100 g of the sample was weighed in a 100-mL
corked conical flask, and an appropriate amount of methylene blue
test solution (mass concentration of 1.5 g/L) was added. Once the
sample was completely wet, it was placed on a shaker at constant tem­
perature and shaken for 20 min and then filtered through a medium-
speed qualitative filter paper. Subsequently, the absorbance of the
filtrate was measured using the UV-2600 spectrophotometer (Shanghai
Tian Mei Scientific Instrument Co., Ltd., China) at a wavelength of 665
nm. The absorbance of the filtrate was compared with that of the copper
sulfate standard solution (4.000 g of crystalline copper sulfate
Cu2SO4⋅5H2O was weighed and dissolved in 1000 mL of water). When
the absorbance of the filtrate was lower than that of the copper sulfate
standard solution, the number of milliliters of the methylene blue test
solution used was denoted as the methylene blue adsorption value of the
sample.
The mass concentration of phosphoric acid solution was confirmed
according to the adsorption capacity of the activated carbon. The
carbonization temperature (300, 400, 500, 600, and 700◦ C) and
carbonization time (60, 90, 120, 150, and 180 min) were confirmed by
the same treatment.
Entropy is one of the metrics for the diversity or uniformity of a
microstate in the theory of thermodynamics. Information entropy is a
measure of the degree of information disorder. The larger the informa­
tion entropy, the higher the degree of information disorder, and the
smaller the utility value (Ma and Ma, 2018). Compared with the sub­
jective weighting methods, such as the Delphi method and analytic hi­
erarchy process, the entropy weight method uses the difference between
information to assign weights and obtains the optimal weight from the
F. Zhang et al. Industrial Crops & Products xxx (xxxx) xxx

actual data of each sample, which is more objective (Vidal et al., 2011). Table 1
This method is transparent and reproducible. According to the literature Yield and methylene blue adsorption value of activated carbon prepared with
reports (Suh et al., 2011; Fadlallah et al., 2013; Siddiqui and Tyagi, different phosphoric acid concentration under material-liquid ratio 1:2 and
2018; Yi et al., 2018), the information entropy weight method was carbonization at 500℃ for 120 min. The comprehensive score M is calculated by
employed for the selection of the best process of activated carbon Eq. 6.
preparation in this study. Phosphoric acid Yield / Methylene blue adsorption / M
concentration / % % (mL/0.1 g)

2.3. BET and BJH test for activated carbon from BWA 30 58.30 4.0 0.0701
40 54.50 4.5 0.0731
50 51.93 5.5 0.0818
The specific surface area and pore-size volume were measured using
60 49.90 4.0 0.0658
the KUBO-X1000 analyzer (Beijing Biod Electronic Technology Co., Ltd., 70 58.41 2.0 0.0501
China). The specific surface area of activated carbon was calculated
from the nitrogen adsorption isotherm using the Brunauer-Emmett-
Teller (BET) equation (Brunauer et al., 1938). The pore-size distribu­
Table 2
tion was simulated using the Horvath-Kawazoe (HK) theory and Yield and methylene blue adsorption value of activated carbon prepared with
Barrett-Joyner-Halenda (BJH) equation (Barrett et al., 1951; Joyner different carbonization temperature under material-liquid ratio 1:2, 50 %
et al., 1951; Horváth and Kawazoe, 1983). phosphoric acid concentration and carbonization 120 min. The comprehensive
score M is calculated by Eq. 6.
2.4. Adsorption of phenolic wastewater by activated carbon Carbonization Yield / Methylene blue adsorption / M
temperature / ℃ % (mL/0.1 g)
Five samples were prepared using varying concentrations of 150 mL
300 29.67 3.0 0.0453
phenol solution (mass concentrations of 200, 405, 705, 1005, and 1395 400 57.54 4.0 0.0697
mg/L) and 0.2 g activated carbon in 250 mL corked conical flasks. 500 51.40 5.0 0.0766
Then, the samples were placed on a shaker and then shaken 600 35.63 3.5 0.0534
constantly at 150 rpm at different temperatures. Subsequently, sampling 700 25.95 2.0 0.0334

and analysis of the mass concentration of phenol in a simulated waste­

water at different times were conducted.
High-performance liquid chromatography analysis of phenol con­ Table 3
centration was conducted on a high-performance liquid chromatograph Yield and methylene blue adsorption value of activated carbon prepared with
LC-20A (Shimadzu Co., Japan) equipped with a C18 column (25 cm different carbonization time under material-liquid ratio 1:2, 50 % phosphoric
acid concentration and carbonization at 500℃. The M comprehensive score is
×4.6 mm, 5 μm). An elution system using a mobile phase composed of
calculated by Eq. 6.
30 % water (A) and 70 % methanol (B) was followed. The flow rate was
set to 1 mL/min, and the injection volume was 10 μL. The detected Carbonization time / Yield / Methylene blue adsorption / (mL/ M
min % 0.1 g)
wavelength was monitored at 254 nm. The real-time adsorption amount
qt (mg/g) was calculated using Eq. (1) in the light of the results of phenol 60 51.44 5.0 0.0766
concentration before and after adsorption by the activated carbon. 90 53.04 6.0 0.0874
120 54.44 5.5 0.0831
When the phenol concentration was closed to no changes with time, the 150 45.83 5.0 0.0737
adsorption was considered to have reached equilibrium. The equilib­ 180 38.43 4.0 0.0599
rium adsorption amount qe (mg/g) was calculated using Eq. (2).

qt =
V × (ρ0 − ρt )
(1) phosphoric acid concentrations, carbonization temperature, and
W carbonization time are presented in Tables 1–3.
The best process for the preparation of activated carbon based on the
V × (ρ0 − ρe )
qe = (2) information entropy weight theory was determined. The original index
W

⃒ ⃒
⃒ 58.3 54.5 51.93 49.9 58.41 29.67 57.54 51.4 35.63 25.95 51.44 53.04 54.44 45.83 38.43 ⃒
X = ⃒⃒ ⃒
4.0 4.5 5.5 4.0 2.0 3.0 4.0 5.0 3.5 2.0 5.0 6.0 5.5 5.0 4.0 ⃒

In Eqs. (1) and (2), ρ0 (mg/L) denotes the initial phenol concentra­ matrix (X) was established using the yield of activated carbon and
tion before adsorption; ρt (mg/L), the phenol concentration at an methylene blue adsorption value as evaluation indicators.
adsorption in real time; ρe (mg/L), the phenol concentration at
adsorption equilibrium time; W (g), the quantity of added activated
carbon; and V (L), the volume of phenol solution. A probability matrix (Pij )mn was converted from the original matrix,
where m and n denote the serial number of row and column respectively.
3. Results and discussion /∑
n
Pij = Xij Xij (3)
3.1. The best process for the preparation of activated carbon from BWA j=1

In Eq. (3), Pij denotes to probability of experiment order number (j)

The yield and methylene blue adsorption value of activated carbon
under evaluation indicator (i).
prepared with a fixed material-to-liquid ratio of 1:2, different

3
F. Zhang et al.
⃒ ⃒
⃒ 0.0814 0.0761 0.0725 0.0697 0.0815 0.0414 0.0803 0.0717 0.0497 0.0362 0.0718 0.0740 0.0760 0.0640 0.0536 ⃒
P = ⃒⃒
0.0635 0.0714 0.0873 0.0635 0.0317 0.0476 0.0635 0.0794 0.0556 0.0317 0.0794 0.0952 0.0873 0.0794 0.0635 ⃒
The information entropy (Hi ) of each index was calculated as Hi ＝
[0.9910, 0.9845] using Eq. (4). The weight coefficient (Wi ) was calcu­
lated as Wi ＝[0.3682, 0.6318] using Eq. (5). The comprehensive score
(M) was calculated after weighting the data of the probability matrix
(Pij )mn using Eq. (6), the results are shown in Tables 1–3.
∑
n
Hi = − k Pij InPij , k = 1/Inn (4)
j=1
Wi = ∑
1 − Hi
(5)
m
(1 − Hi )
j=1
Mi = P1i W1 + P2i W2 (6)
According to the comprehensive score (M), the best process for the
preparation of activated carbon from BWA involves phosphoric acid
concentration of 50 %, carbonization temperature of 500℃, and
carbonization time of 90 min. Under these conditions, the yield of
activated carbon from BWA was 53.04 %, and the methylene blue
adsorption value was 6.0 mL/0.1 g.
3.2. Specific surface area and pore size distribution of activated carbon
Fig. 1 presents the nitrogen adsorption and desorption isotherm of
activated carbon from BWA, which belongs to type I (Thommes et al.,
2015), where in the curves are almost coincident and have no hysteresis.
From the figure, it can be seen that the pore is of wedge type or cone type
(Duong, 2000).
The adsorption in a wedge pore exhibits richer features than that on a
planar substrate. This is because the apex acts as a strong site for
adsorption resulting from the overlap of potentials exerted by the re­
gions of the pore walls close to the apex (Loi et al., 2020). Conversely, in
a wedge pore, in addition to the wetting transition on the surfaces, the
adsorbate can fill the pore space or cluster at apices at the bulk coexis­
tence pressure P0 (Zeng et al., 2015; Loi et al., 2020). It can also be seen
that the adsorption material that is of wedge type or cone type exhibits
better adsorption performance.
Fig. 1. Isotherms of nitrogen adsorption and desorption.
4
Industrial Crops & Products xxx (xxxx) xxx
⃒
Table 4 presents the following characteristics of activated carbon
from BWA: BET surface area, micropore surface area, Langmuir surface
area, total pore volume, micropore volume, and average pore size. The
BET surface area and average pore size were 390.89 m2 g− 1 and 4.7 nm,
respectively. It is worth noting that the average pore size reflects the
ability of the adsorbed molecules to diffuse to the adsorption sites of
activated carbon (Lorenc-Grabowska, 2016; Oginni et al., 2019). The
effective molecular diameter for phenol was 0.75 nm, which was smaller
than the average pore size of the activated carbon. This indicates the
suitability of activated carbon prepared from BWA for phenol
adsorption.
The comparison of the carbon product from this work with those of
the others using the same activation method (phosphoric acid activa­
tion) is presented in Table 5, whereas Table 6 presents the comparison
between the properties of activated carbon prepared using various types
of activation methods. It can be seen that the conditions of this works for
the preparation of activated carbon from BWA are reasonable and that
the prepared activated carbon exhibits a high BET specific surface area,
total pore volume, and yield. This indicates that the use of industrial
crop waste material BWA to prepare activated carbon has a high
development potential.
3.3. Phenol adsorption behaviors of activated carbon from BWA
The adsorption curves of activated carbon from BWA on the indi­
vidual initial concentrations of phenol at different temperatures are
presented in Fig. 2. From the figure, it can be seen that the adsorption
amount rapidly decreases in the initial stage, and the adsorption curves
gradually smooth with the extension of the adsorption time at the
temperatures of 25, 35, and 45◦ C. When the adsorption time was as long
as 4 h, adsorption reached equilibrium, wherein the adsorption amount
was virtually unchanged. Therefore, the equilibrium time for phenol
adsorption on activated carbon from BWA was 4 h.
The calculated phenol initial concentration values versus equilib­
rium adsorption amount of activated carbon from BWA are plotted in
Fig. 3. The plot indicates that the increase in the equilibrium adsorption
amount is dependent on the temperature and initial phenol
concentration.
3.4. Thermodynamics of phenol adsorption on activated carbon from
BWA
Studying the adsorption isotherm of phenol solution on the activated
carbon from BWA can conclude the law that activated carbon absorbs
phenol, the study can provide important reference for the adsorption
process parameters (Kujawski et al., 2004; Dong et al., 2012;
Wiśniewskia et al., 2012).
Table 4
Result of specific surface area and pore size of activated carbon from BWA.
SBETa (m2 Smicb (m2 SLangmuirc VTotald Vmicroe D Averagef
g− 1) g− 1) (m2 g− 1) (cm3 g− 1) (cm3 g− 1) (nm)
390.89 474.26 429.50 0.3826 0.1686 3.92
a
BET (Brunauer-Emmett-Teller) surface area.
b
Micropore surface area.
c
Langmuir surface area.
d
Total pore volume, measured at P/P0 = 0.995.
e
Micropore volume.
f
Average pore diameter of absorbents.
F. Zhang et al. Industrial Crops & Products xxx (xxxx) xxx

Table 5
Comparison of phosphoric acid activated carbon obtained from this work and other reports.
Description This work Khan et al., 2016 Abatal et al., 2020 Khellouf et al., 2020 Shah et al., 2020

Raw material bark waste of Acacia mangium brown linseed bark of H. campechianum cypress cones sawdust of
Melia azedarach
Activation 500℃ for 90min 700℃ for 2 h 500℃ for 1 h 500℃ for 4 h 400℃ for 30 min
Impregnation ratio 1:2, with 50 % acid 1:1.5, with 85 % acid 1:2, with 85 % acid 1:1, with 85 % acid 1:2, with 85 % acid
Yield (%) 53.04 41.5 45 – –
BET surface area (m2 g− 1) 390.89 282.62 181.49 379.51 293.13
Total pore volume (cm3 g− 1) 0.3826 0.0935 0.09396 0.204 0.15
average pore size (nm) 3.92 5.230 2.07 2.21 2.033

isotherm adsorption equation. In the Freundlich adsorption isotherm

Table 6
model, the parameter KF was related to the phenol adsorption capacity
Comparison of various types of activated carbon obtained from this work and
of activated carbon from BWA. As the adsorption temperature increased,
other reports.
the KF values gradually decreased, indicating that the capacity of acti­
Description This work Ahmad Rashidi Ravichandran Yek vated carbon to adsorb phenol decreased with the increase in temper­
et al., and et al., 2018 et al.,
2014 Yusup, 2020
ature. This is consistent with the curve trend demonstrated in Fig. 3, in
2017 which the equilibrium adsorption amount of phenol on activated carbon
decreases as the temperature increases. From the experimental results,
Raw bark waste Date palm waste of orange
material of Acacia Fronds kernel Casuarina peel we found that the adsorption was an exothermic process, indicating that
mangium Biomass shell equisetifolia waste a lower temperature is conducive to adsorption. The n values obtained in
fruit this study were all greater than 2. This means that phenol was easily
Activating phosphoric Potassium carbon Zinc chloride Steam adsorbed by activated carbon from BWA (Sharma et al., 2016; Nasci­
agent acid hydroxide dioxide
Activation 500℃ for 400℃ for 850℃ 700℃ for 1 h 800℃
mento and Masini, 2018).
90min 3h for 1 h for 15
min 3.5. Kinetics of phenol adsorption on the activated carbon from BWA
Yield (%) 53.04 39.0 25.15 56.48 31
BET 390.89 250.25 367.8 335.08 305.1
To elucidate the kinetics of phenol adsorption on the activated car­
surface
area (m2 bon from BWA, the data presented in Fig. 2 were fitted by the McKay
g− 1) second-order model (Liu et al., 2015), and the results are presented in
Total pore 0.3826 0.082 0.2199 0.418 0.26 Fig. 5.
volume The values of qt and qe,c at different temperatures were utilized for
(cm3
g− 1)
the model fitting. The linearized form of each model was used, which
average 3.92 1.417 2.392 7.568 1.9 can be expressed as follows:
pore size
t 1 t
(nm) = + (9)
qt K2 q2e,c qe,c

The thermodynamic aspects of phenol adsorption behaviors on
activated carbon were investigated through the analysis of phenol
adsorption data at various temperatures (25, 35, and 45◦ C) and initial
phenol concentrations (200, 405, 705, 1005, and 1395 mg/L) according
to section 2.4 of this works.
The results are presented in Fig. 2. In liquid-phase adsorption, the
Freundlich adsorption isotherm formula[Eq. (7)] is generally considered
to be suitable for the adsorption of organic compounds on an aqueous
solutions by activated carbon (Chern and Chien, 2002; Chaudhary et al.,
2003; Jadhav and Srivastava, 2013). This formula can be converted to a
linearization formula[Eq. (8)]. Therefore, the Freundlich adsorption
isotherm formula was fitted to the adsorption process. The fitted results
are presented in Fig. 4, and the fitted model parameters are listed in
Table 7.
Freundlich adsorption isotherm formula : qe = KF ρe 1/n
1
Linearization formula : lnqe = lnKF + lnρe
n demonstrates that the following three stages can be involved in the
In Eqs. (7) and (8), KF denotes the adsorption capacity of activated
carbon; n, the Freundlich constant; qe (mg/g), the equilibrium adsorp­
tion capacity; and ρe (mg/g), the concentration of phenol solution at
adsorption equilibrium time.
Table 7 presents the adsorption equilibrium constant for each
isotherm data obtained at various temperatures. It was calculated using
the linearization Freundlich model. The correlation coefficients of the
linear fitting results were very close to 1 (R2 > 0.96), indicating that the
adsorption thermodynamic was well simulated using the Freundlich
In Eq. (9), qt and qe.c denote the amount of adsorbate uptake (mg) per
1 g of adsorbent at each adsorption time and equilibrium state, respec­
tively. K2 denotes the second-order adsorption rate constant of the
equations, and t (min) denotes the adsorption time. The parameters of
the adsorption kinetic model obtained by the fitting are presented in
Table 8–10. The adsorption kinetic of phenol adsorption on activated
carbon from BWA flowed McKay second-order adsorption kinetic
equation, which the correlation coefficients were 0.9985− 0.9999 (close
to 1) at 25, 35, and 45◦ C.
Although the McKay second-order model can describe the kinetic
data of adsorption on activated carbon from BWA by the fitting, it did
not demonstrate the adsorption mechanism. The Weber and Morris in­
ternal diffusion model is often used to analyze the adsorption rate
controlling steps (June et al., 2020). The experimental data were ob­
tained using the Weber and Morris model.
(7) From Fig. 6, it can be seen that the fitting curve of the intraparticle
diffusion model for activated carbon adsorption of phenol at different
(8) temperatures consists of three straight lines with different slopes. This
phenol adsorption process on porous adsorbents in an aqueous phase:
(1) transport of phenol from the bulk solution to the external surface of
adsorbents, (2) diffusion of phenol into inner pores (intraparticle
diffusion), and (3) adsorption of phenol on the internal surface of pores
(Gercel et al., 2007).
The adsorption mechanism of which kinetic is influenced by the
intraparticle diffusion can be interpreted based on the plot of qt vs the
square root of time. It can be expressed by Eq.(10) (June et al., 2020).

5
F. Zhang et al. Industrial Crops & Products xxx (xxxx) xxx

Fig. 2. The adsorption curves of activated carbon from BWA on individual initial concentrations of phenol. (A), (B) and (C) correspond to various temperatures 25,
35, and 45℃.

Fig. 3. Relationship between phenol initial concentration (mg⋅L− 1) and equi­

librium adsorption amount (mg⋅g-1). Fig. 4. Linearization formula of Freundlich adsorption isotherm.

diffusion rate constants Kp and C values in Tables 8–10. The C values

qt = Kp t1/2 + C (10)
Where Kp (mg/g × min1/2) denotes the rate constant of the Weber and
Morris model, and C (mg/g) denotes a constant related to the boundary
layer thickness (the higher the C values, the greater the influence of the
limiting boundary layer).
The second segment of the straight line in Fig. 6 fits the intraparticle
were greater than 0, and some R2 values were not close to 1, indicating
that the diffusion in the activated carbon particles was not the only
adsorption process. It is possible that there are other spontaneous dy­
namic control processes. The linear curve of each plot presented in Fig. 6
indicates that the external surface absorption process occurs rapidly and
the overall adsorption rate is dominantly controlled by the intraparticle

6
F. Zhang et al. Industrial Crops & Products xxx (xxxx) xxx

Table 7 4. Conclusions
Fitting results of isothermal equation for phenol adsorption by activated carbon.
temperature/℃ Adsorption isotherm equation KF n R2 The bark waste after the extraction of industrial tannins from Acacia
mangium can be used to prepare activated carbon. The activated carbon
25 qe = 10.4855ρ0.303
e 10.4855 3.3054 0.9703
35 qe = 8.6827ρ0.296
e 8.6827 3.3836 0.9742 yield and value were as weight coefficients using the information en­
45 qe = 0.427
3.2128ρe 3.2128 2.3402 0.9921 tropy weight method to select the best process employing the phos­
phoric acid activation method. The optimized conditions for the
*qe (mg/g) means the equilibrium adsorption capacity.
*ρe (mg/L) means the phenol concentration at adsorption equilibrium time.
preparation of activated carbon are as follows: phosphoric acid con­
*KF means the adsorption capacity of activated carbon. centration of 50 %, carbonization temperature of 500◦ C, and carbon­
*n means the Freundlich constant. ization time of 90 min. The performance of methylene blue adsorption
on activated carbon from BWA indicated that activated carbon had the
diffusion of activated carbon. Phenol molecules can diffuse into the same absorption effect on phenol wastewater. The phenol adsorption
inner pores of activated carbon either at aqueous solution states or at behaviors of activated carbon from BWA and its thermodynamic and
adsorbed states. The major driving force of both cases was the concen­ kinetic characteristics were further investigated.
tration gradient of phenol molecules (at aqueous solution or adsorbed The thermodynamic studies revealed that the Freundlich adsorption
states) from the exterior to the interior of the pores. isotherm model can well describe the phenol adsorption process on

Fig. 5. Fitting curve of McKay secondary adsorption kinetics with different initial concentrations. (A), (B) and (C) correspond to various temperatures 25, 35,
and 45℃.

Table 8
The fitted parameters of adsorption kinetic models with different initial concentrations (25℃).
ρ0 /(mg/L) qe/(mg/g) McKay Weber and Morris

k2/(g/(mg•min)) qe,c /(mg/g) R2 kp /(mg/(g min1/2 ))

•
C/(mg/g) R2

3
205 47.55 3.22 × 10− 48.17 0.9998 1.24 32.95 0.8527
3
405 60.23 4.14 × 10− 60.90 0.9999 1.82 43.51 0.8207
3
705 68.88 3.65 × 10− 69.25 0.9999 1.75 51.66 0.9015
3
1005 79.94 3.69 × 10− 80.26 0.9999 1.90 61.43 0.8841
3
1395 96.92 1.65 × 10− 97.09 0.9985 2.07 69.21 0.8802

*ρ0 means the initial phenol concentration before adsorption.

*qe means the equilibrium adsorption capacity.
*k2 means the second-order adsorption rate constant of the equations.
*qe,c means the adsorbate uptake (mg) per one gram of adsorbents at equilibrium state.
*kp means the rate constant of the Weber and Morris model.
*C means the constant related to the boundary layer thickness.

7
F. Zhang et al. Industrial Crops & Products xxx (xxxx) xxx

Table 9
The fitted parameters of adsorption kinetic models with different initial concentrations (35℃).
ρ0 /(mg/L) qe/(mg/g) McKay Weber and Morris
2
k2/(g/(mg•min)) qe,c /(mg/g) R kp /(mg/(g min1/2 ))
•
C/(mg/g) R2

3
205 36.86 8.58 × 10− 36.83 0.9997 0.05 34.01 − 0.917
3
405 51.28 3.16 × 10− 51.57 0.9994 1.52 34.32 0.9998
3
705 58.76 3.09 × 10− 58.75 0.9985 2.16 37.24 0.9608
3
1005 64.64 5.61 × 10− 65.02 0.9999 1.68 49.99 0.9377
3
1395 70.91 4.69 × 10− 70.97 0.9998 0.61 62.06 0.7547

*ρ0 means the initial phenol concentration before adsorption.

*qe means the equilibrium adsorption capacity.
*k2 means the second-order adsorption rate constant of the equations.
*qe,c means the adsorbate uptake (mg) per one gram of adsorbents at equilibrium state.
*kp means the rate constant of the Weber and Morris model.
*C means the constant related to the boundary layer thickness.

Table 10
The fitted parameters of adsorption kinetic models with different initial concentrations (45℃).
ρ0 /(mg/L) qe/(mg/g) McKay Weber and Morris

k2/(g/(mg•min)) qe,c /(mg/g) R2 kp /(mg/(g min1/2 ))

•
C/(mg/g) R2

205 27.82 20.48 × 10− 3 27.88 0.9999 0.21 25.19 0.9926

405 39.58 5.92 × 10− 3 39.97 0.9997 0.61 31.47 0.9982
705 52.82 4.24 × 10− 3 53.19 0.9990 0.68 44.28 0.9993
1005 59.42 3.74 × 10− 3 59.84 0.9998 1.51 44.39 0.9999
1395 66.98 2.65 × 10− 3 66.98 0.9989 0.75 53.90 0.1696

*ρ0 means the initial phenol concentration before adsorption.

*qe means the equilibrium adsorption capacity.
*k2 means the second-order adsorption rate constant of the equations.
*qe,c means the adsorbate uptake (mg) per one gram of adsorbents at equilibrium state.
*kp means the rate constant of the Weber and Morris model.
*C means the constant related to the boundary layer thickness.

Fig. 6. Fitting curve of Weber and Morris adsorption kinetics with different initial concentrations. (A), (B) and (C) correspond to various temperatures 25, 35,
and 45℃.

8
F. Zhang et al.
activated carbon from BWA. The thermodynamic parameters, such as KF
and n, were calculated using the linearization formula of the Freundlich
model. It was found that the calculated KF values gradually decreased as
the temperature increased, indicating that the capacity of activated
carbon to adsorb phenol decreased with the increase in temperature.
The n values obtained in this study were all greater than 2. This means
that phenol was easily adsorbed by activated carbon from BWA. The
amount of phenol adsorption at equilibrium decreased as the tempera­
ture increased. This phenomenon can be attributed to the adsorption
being an exothermic process.
The kinetic behaviors of the phenol adsorption process on activated
carbon from BWA can be described using the McKay second-order model
and Weber and Morris model. As the correlation coefficients are
0.9985− 0.9999 (close to 1) at 25◦ C, 35◦ C, and 45◦ C, the phenol
adsorption process flowed McKay second-order adsorption kinetic
equation. The mechanism of the phenol adsorption process on activated
carbon from BWA was further explained by the Weber and Morris
model. The C values were greater than 0, and some R2 values were not
close to 1. These values were calculated based on the Weber and Morris
model, indicating that the diffusion in the activated carbon particles was
not the only adsorption process. It is possible that there are other
spontaneous dynamic control processes.
CRediT authorship contribution statement
Feihu Zhang: Investigation, Data curation, Writing - original draft.
Sheng Zhang: Conceptualization. Lei Chen: Investigation, Validation,
Writing - review & editing, Resources. Zilei Liu: Investigation, Formal
analysis. Junjie Qin: Investigation, Methodology.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
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