Journal of Materials Research and Technology 27 (2023) 6900–6911

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Journal of Materials Research and Technology

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

A novel polymer-type binder to decrease bentonite dosage during iron ore

pelletizing: Performance and mechanisms
Yonghe Ma a, Qian Li a, Yan Zhang a, *, Yongbin Yang a, Yinhua Tang b, Tao Jiang a
a
School of Minerals Processing and Bioengineering, Central South University, Changsha, Hunan 410083, China
b
Xinyu Iron and Steel Co., Ltd., Xinyu, Jiangxi 338013, China

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

Keywords: The decrease in the total iron grade of pellets due to bentonite has prompted the search for a non-polluting and
Polymer-type binder alternative binder. While organic binders are considered potential substitutes for bentonite, they cannot fully
Bentonite replace it due to complete decomposition and failure during pellet hardening. Thus, the production of pellets
Iron ore pelletizing
utilizing a composite of organic binder and bentonite has gained significant attention in academia and industry.
Adsorption
In this study, a novel polymer-type binder (PTB) was introduced to minimize bentonite consumption during
green pellet preparation. By regulating the ratio, the addition of just 0.01% PTB can reduce bentonite usage by
1.0% under optimal conditions, all while maintaining excellent pellet quality. Further investigations revealed
that PTB molecules adsorbed on the surfaces of iron concentrate (predominantly magnetite) and bentonite
through hydrogen bonding, electrostatic repulsion, coordination, monodentate chelation and surface complex­
ation, and dissolved into a fibrous structure to bridge the particles together. Moreover, the abundant hydrophilic
groups (-OH, –COOH) in PTB substantially enhanced the water-holding capacity of green pellets, resulting in a
reduced rate of drying dehydration and an elevated shock temperature. This comprehensive study provides
valuable scientific insights into the development and application of composite binders.

1. Introduction
Pelletization is a clean and essential method of producing materials
for iron-making due to its low energy consumption and minimal
pollutant emissions [1–3]. With the "carbon peak and neutrality" back­
ground, increasing the proportion of pellet feed in charge can effectively
reduce carbon emissions in Chinese blast furnace iron-making [4,5].
Therefore, the robust development of pellets to reduce blast furnace
energy consumption and promote low-carbon growth in the steel in­
dustry holds great significance.
The binder is an essential auxiliary material in the production of iron
ore pellets as it controls the properties of both green and hardened
pellets [6]. Currently, bentonite serves as the predominant binder in iron
ore pellet production, typically in dosages ranging from 1.5% to 3.0%
[4,7]. However, excessive use of bentonite can seriously affect pellet
quality due to its main components, SiO2 and Al2O3. It is reported that
the addition of 1% bentonite can decrease the pellet iron grade by 0.4%–
0.6% [8]. Therefore, it is crucial to reduce the bentonite ratio in pro­
duction to increase the pellet iron grade and minimize process con­
sumption. Organic binders are considered superior substitutes for
bentonite due to their high viscosity, significant burn-off, and low re­
sidual properties [9–11]. Presently, researchers have extensively
investigated various organic binders such as coal tar, starch, dextrin,
guar gum, dairy products, honey, and sodium carboxymethyl cellulose
(CMC), all characterized by high molecular weight polymers with
multifunctional groups, so categorizing them as polymer-type binders
(PTBs) [12–15]. The incorporation of PTBs in pellets results in a lower
gangue content and a porous structure, facilitating rapid gas diffusion
during reduction. Consequently, the energy and melt consumption of the
iron-making process can be significantly decreased [16]. However, the
utilization of PTBs alone presents an inevitable drawback: low cold
compressive strength of preheated and roasted pellets. This is attributed
to (i) the low decomposition temperature of PTBs, leading to burning
decomposition and bonding failure during the preheating stage; (ii) the
insufficient organic binder slag, resulting in inadequate slag bonding
consolidation of the roasted pellets [16,17]. This constitutes a technical
barrier restricting the large-scale industrial application of PTBs. In
summary, both bentonite and PTBs have inherent limitations when used
independently.
Therefore, to minimize the usage of bentonite in pellet production,

* Corresponding author.
E-mail address: yanzhang301527@163.com (Y. Zhang).

https://doi.org/10.1016/j.jmrt.2023.11.134
Received 27 August 2023; Received in revised form 12 November 2023; Accepted 16 November 2023
Available online 17 November 2023
2238-7854/© 2023 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-
nc-nd/4.0/).
Y. Ma et al.
researchers have synergistically combined PTBs with bentonite [8,18,
19]. A study has demonstrated that the chemical interaction between
Alcotac® CS (a PTB) and bentonite greatly enhances the bonding
properties. Adding just 0.02% Alcotac® CS reduces the necessary
bentonite dosage from 1.8% to 1.0% while significantly improving the
quality of the resulting green pellets, particularly the drop number,
which increased from 4.2 to 8.2 times/0.5 m [8]. Moreover, humic
acid-modified bentonite (HAMB) displayed remarkably enhanced
bonding, with the drop number of green pellets exceeding that of 1.0%
bentonite when using only 0.5% HAMB. However, the structure and
thermal stability of bentonite were altered by humic acid, resulting in
reduced thermal stability of HAMB. Consequently, the drying tempera­
ture of green pellets containing HAMB should not exceed the specified
threshold [20]. Another study indicates that expanded starch can
decrease the required amount of bentonite in pellet production. This
effect is attributed to the efficient adsorption between –COOH or –OH
groups in expanded starch and the surface of bentonite sheets, leading to
improved surface electronegativity and hydrophilicity of bentonite [21].
Scholars have found that using 1.2% bentonite and 0.028% organic
binder (P) in composite binder pellets with higher drop number (6.2
times/0.5 m), compressive strength (14.5 N/P), and shock temperature
(542 ◦ C) when compared to 2.0% bentonite pellets, while simulta­
neously reducing bentonite consumption by 0.8% [22]. Previous in­
vestigations have demonstrated the effectiveness of various PTBs,
including expanded starch, humic acid, sodium lignin sulfonate, and
sodium carboxymethyl cellulose, in declining bentonite consumption.
However, the reduction in bentonite consumption by PTB in prior
studies is modest (approximately 0.5%–0.8%), with less elaboration on
the interaction mechanism between PTB, bentonite, and iron ore
concentrate. Additionally, the specific contributions of PTB and
bentonite to the green pellet quality index remain ambiguously
expressed.
Herein, this study introduced a novel PTB (as functional component)
and bentonite (as dispersion carrier) for pelletizing to significantly
reduce the consumption of bentonite and investigate the behavior and
mechanisms of PTB on the quality of green pellets. The objectives of this
work are to (i) establish the optimal bentonite to PTB ratio for improved
bonding performance, (ii) investigate the impact of PTB on the quality
and drying behavior of green pellets, and (iii) elucidate the synergistic
mechanism between PTB and bentonite in enhancing pellets properties.
2. Materials and methods
2.1. Materials
The materials utilized in this study include two types of iron con­
centrates (named A and B), bentonite, and PTB. The iron concentrates
and bentonite were obtained from Hubei Jinshenglan Metallurgical
Technology Co., Ltd, China, while PTB was provided by the School of
Minerals Processing and Bioengineering, Central South University,
Changsha, China. Detailed characteristics of materials are described in
Section 3.1.
2.2. Methods
2.2.1. High-pressure grinding roll pretreatment
To ensure consistent Blaine number for different raw material ratios
and minimize the impact of poor ballability concentrate on the
agglomeration of the mixes, a high-pressure grinding roll (HPGR) was
utilized to enhance their particle size distribution and surface activity.
The HPGR is equipped with rollers measuring 250 mm in diameter and
120 mm in length, controlled by a hydraulic drive system. Throughout
the experiment, we maintained a constant roller pressure of 32.4 KN and
38.5 KN, respectively, by adjusting the hydraulic drive system while
keeping the feed rate consistent. This resulted in corresponding pres­
sures of 1.0 MPa and 1.2 MPa on the cross-section of the rollers,
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Journal of Materials Research and Technology 27 (2023) 6900–6911
respectively. Furthermore, the corresponding Blaine number of the
discharged material were 1726.34 cm2/g and 1973.09 cm2/g, as
depicted in Fig. 1.
2.2.2. Pelletizing
PTB was compounded with bentonite in a predetermined ratio and
manually mixed with the discharge after HPGR. Subsequently, pellet­
izing was conducted in a disc pelletizer with a diameter of 1000 mm,
side height of 200 mm, and inclination angle of 45◦ using 5 kg of mixture
each trial (Fig. 1). After pelletizing for 12 min, qualified green pellets
within 10–12 mm were screened out and tested drop number,
compressive strength, and shock temperature. The drop number was n-1
times of green pellets falling freely from a 0.5 m height until rupture,
with a minimum requirement for this work of ≥4 times/0.5 m.
Compressive strength was determined as the maximum crushing pres­
sure that green pellets could withstand. The shock temperature was
defined as the maximum temperature at which exactly two out of the 50
green pellets burst when exposed for 5 min in a shaft furnace with 1.5 m/
s air velocity. It is noteworthy that all of the above indicators were
measured three times for accuracy.
2.2.3. Drying experiments
The drying experiment of green pellets was taken in a vertical-tube
furnace of Ø 650 × 1000 mm (Fig. 1). The tube was filled with
alumina ceramic balls for heat storage, resulting in the rapid elevation
and maintenance of the furnace airflow temperature at a preset value.
Subsequently, 500 g of green pellets were placed into a steel cup
measuring Ø 55 × 195 mm, featuring 60 uniform holes at the bottom.
These pellets were exposed to the furnace for 5 min, and the cup was
promptly removed every 20 s. Weight changes were recorded to calcu­
late the corresponding drying and dehydration rates, with the calcula­
tion formulas as follows:
Δm
v= (1)
t
Δm
φ= ×100% (2)
500ω
where Δm is the amount of pellet dehydration (g), t is time (s), v is the
drying rate (g/s), ω is the moisture content of green pellets (g), and φ is
the dehydration rate (wt.%). It was noted that the compressive strength
measurement of the dried pellets followed that of the green pellets.
2.2.4. Analysis and characterization methods
The sample preparation, analytical methods, instruments, and pa­
rameters are described in detail in Text S1.
3. Results and discussion
3.1. Analysis of raw material properties
3.1.1. Iron concentrates
The chemical compositions of iron concentrate A and B are detailed
in Table 1. Both A and B represented high-grade iron concentrates with
grades exceeding 64%, although A contained a significantly higher FeO
content (31.36%) compared to B (0.40%). The primary gangue
component in both is SiO2, with levels of 6.51% and 4.28%, respectively.
XRD analysis unequivocally demonstrated that A is composed of
magnetite, whereas B is characterized as hematite (Fig. 2(a)). Further­
more, A with a finer average particle size (d50) and larger Blaine number
is a superior feed material, while the coarser d50 (996.011 μm) and a
smaller Blaine number (1180.01 cm2/g) are found for B (Fig. 2(b)).
Therefore, optimizing the particle size distribution of the mix is essential
if B occupies a larger proportion.
Y. Ma et al. Journal of Materials Research and Technology 27 (2023) 6900–6911

Fig. 1. Schematic diagram of the experimental flow.

Table 1
Chemical compositions of iron concentrates (wt.%).
Sample TFe FeO SiO2 CaO MgO Al2O3 MnO P TiO2 Cu LOI

A 65.59 31.36 6.51 0.48 0.37 0.66 0.059 0.029 0.10 0.01 − 2.47
B 64.32 0.40 4.28 0.24 0.12 0.73 0.33 0.060 0.078 0.037 2.56

LOI-loss on ignition.

3.1.2. Binders High-temperature thermodestruction and functional groups of PTB

Table 2 shows the chemical composition of bentonite, and its XRD
pattern and particle size distribution are presented in Fig. 3(a-b). Its
main mineral compositions are montmorillonite, quartz, and andesine,
exhibiting a d50 of 5.814 μm.
PTB was synthesized by our research group through the modification
of commercial polyethylene oxide with a relative molecular weight of
approximately 7 million, and the detailed preparation process can be
found in the Chinese patent ZL202110590600.8 [23]. The viscosity of a
1% PTB solution measured approximately 30 mPa⋅s. The proximate
analysis and elemental content of PTB are shown in Table 3. Notably, it
exhibits high carbon and oxygen contents (41.63% and 29.38%) but low
levels of H, N, and S, indicating a negligible environmental impact. The
moisture (Mad), ash (Aad), volatile fraction (Vdaf), and fixed carbon
(FCad) contents were determined as 16.26%, 26.64%, 34.82%, and
22.29%, respectively, demonstrating little effect on the total iron grade
of pellets.
were characterized by Thermogravimetry and FTIR (Fig. 3(c–d)). The
initial weight loss stage was attributed to the removal of free water,
resulting in a slight endothermic peak in the DSC curve. Subsequently,
the TG curve showed a 5.51% reduction in weight at 188.8 ◦ C, coin­
ciding with an exothermic peak in the DSC curve. This observation
implied oxidative degradation of PTB. With rising temperature, there
was a progressive escalation in both heat release and weight loss rates.
Notably, a substantial 50.32% weight loss in the TG curve indicated the
destruction of chemical bonds, functional groups, and the organic
combustion of the sample. At 753.1 ◦ C, dominant reactions involved the
gasification and combustion of the residual fixed carbon, as evidenced
by the intense exothermic peak in the DSC curve. The residual sample
was 25.34%, aligning with the proximate analysis results.
According to the FTIR analysis, the characteristic peaks of PTB at
3349-2892, 1578, 1381, 1096-1034, 842, and 538 cm-1 were observed,
which were due to the vibration of –OH, C=C, and the deformation

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Y. Ma et al. Journal of Materials Research and Technology 27 (2023) 6900–6911

(a) (b)16 Iron concentrate A (d50 )

Iron concentrate B 3O4 SiO2
Fe2O3 FeO(OH) Iron concentrate B (d50 )
2000 1888.08

Volume frequency (%)

12

Blaine number (cm2/g)

Intensity (a.u.)

1600

1200 1180.01
8

800
Iron concentrate A
4 400
A B
Sample

0
10 20 30 40 50 60 70 80 0.1 1 10 100 1000
2 (°)

Fig. 2. (a) XRD patterns; (b) Particle size distribution and Blaine number of iron concentrates.

3.2. Preparation of green pellets under different conditions

Table 2
Chemical composition of bentonite (wt.%).
Bentonite serves as the control binder, necessitating a study of the
TFe SiO2 Al2O3 CaO MgO K2O Na2O LOI minimum bentonite dosage required for the preparation of qualified
2.10 65.00 15.50 2.31 1.98 1.87 3.28 7.89 green pellets. The purpose of HPGR pretreatment is to standardize the
Blaine number across feed materials with varying ratios, facilitating
result comparability. In this section, the optimal Blaine number of the
vibration of –OH, Si–O–Si, Fe–O, and Si–O–Al, respectively [24–26]. mix and HPGR feed moisture were first determined. Subsequently, the
Therefore, PTB primarily consisted of polyfunctional (-OH, –COOH, and potential of PTB in reducing bentonite usage and its influence on the
C=C, etc.) polymer molecules with minimal inorganic components. performance of green pellets was explored across various raw material
ratios. Unless otherwise specified, this study employs pelletizing mix
ratios of 65% A and 35% B, determined based on the actual production
ratios of the feeder pelletizing plant.

(a) (b) 7 100

Montmorillonite Volume frequency
Quartz 6 Cumulative volume

Cumulative volume (%)

Volume frequency (%)

Andesine 80
5
Intensity (a.u.)

4 d10 60
d50
3 40
d90
2
20
1

0 0
0 10 20 30 40 50 60 70 80 0.1 1 10 100
2 (°)
(c) 753.1 Endo (d)
100 TG 6
DSC
18.83%
4
Transmittance (%)

80
DSC (mW/mg)

5.51%
2 842
188.8
TG (%)

60 0

69.9 50.32% 3688 538

498.3
40
1034
1096

m(residue)=25.34% 3349 2892 1381

1578
20
200 400 600 800 1000 4000 3500 3000 2500 2000 1500 1000 500
Temperature ( ) Wavenumbers (cm-1)

Fig. 3. (a, b) XRD pattern and particle size distribution of bentonite, and (c, d) TG-DSC curves and FTIR spectra of PTB.

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Y. Ma et al. Journal of Materials Research and Technology 27 (2023) 6900–6911

Table 3
Proximate and elemental analysis of PTB.
Sample Proximate analysis (wt.%) Elemental content (wt.%)

Mad Aad Vdaf FCad C H O N S

PTB 16.26 26.64 34.82 22.29 41.63 4.68 29.38 0.42 0.31

3.2.1. Effect of the Blaine number of the mix and bentonite dosage of green pellets showed minimal fluctuations, remaining with a range of
As mentioned, the minimum Blaine number of the mix by HPGR and 1 N/P. The suitable feed moisture into HPGR was determined to be 9.5%
the necessary bentonite dosage to produce qualified green pellets were after comprehensively assessing its influence on the quality of green
investigated, using bentonite as the reference binder. The results are pellets.
presented in Fig. 4.
The study noted a gradual rise in the drop number, compressive 3.2.3. Effect of PTB composite bentonite
strength, and shock temperature of green pellets as the bentonite dosage As a result of the above study, the effect of PTB composite bentonite
increased in the feed material with a Blaine number of 1726.34 cm2/g. on the quality of green pellets was investigated under optimized con­
However, despite increasing the bentonite addition to 2.2% in this ditions, namely the mix with Blaine number of approximately 1973.09
corresponding HPGR application, the drop number of the resulting cm2/g by HPGR pretreatment, 9.5% feed moisture, and consistent
green pellets remained inadequate, indicating suboptimal mix ball­ pelletizing parameters. As shown in Table 4, the drop number and shock
ability. Conversely, by elevating the roller pressure of the HPGR to temperature of green pellets increased gradually with escalating PTB
achieve a Blaine number of 1973.09 cm2/g for the mixture, a pellet drop dosage, while the compressive strength of green and dried pellets
number of 4.1 times/0.5 m was attained with just 2.0% of bentonite. declined. Despite a PTB ratio of 0.2%, the drop number of the corre­
This achievement can be attributed to the enhanced surface activity, sponding green pellets reached 4.2 times/0.5 m, but the compressive
material amorphization, and micro-fine particle content of the mix strength remained below 10 N/P, failing to meet industrial re­
resulting from higher intensity HPGR [27–29]. It is evident that the quirements. The utilization of PTB composite bentonite notably
necessary bentonite ratio and Blaine number for the feed material to enhanced the quality of pellets, particularly the shock temperature of
prepare high-quality green pellets were 2.0% and 1973.09 cm2/g, green pellets and compressive strength of dried pellets. At bentonite
respectively. additions of ≤0.5%, the rise in PTB ratio minimally affected the drop
number of green pellets. However, with ≥0.8% bentonite addition, an
3.2.2. Effect of feed moisture content into HPGR elevated PTB dosage significantly raised the drop number of green pel­
The efficiency of HPGR is influenced by its process parameters, such lets. This phenomenon was attributed to lower bentonite quantities
as feed moisture content, roll pressure, etc. Therefore, the optimum primarily serving as dispersing carriers for PTB and the severely limited
Blaine number of the mixture can only be attained at a specific moisture dispersion of bentonite components. In contrast, higher dosages of
content [27]. In order to establish the suitable feed moisture content, the bentonite not only worked as inorganic carriers but also synergized with
effect on the quality of green and dried pellets was investigated, using a PTB to improve pellet quality.
2.0% bentonite dosage (Fig. 5). From this, the drop number and shock temperature of green pellets
Generally, a lower feed moisture content in HPGR results in less were substantially increased by the introduction of minor PTB. How­
effective particle embedding, shorter inter-roll intervals, and weaker ever, it harmed the compressive strength of both green and dried pellets,
effects. Conversely, higher feed moisture content will adhere to the roll attributed to the adhesion of PTB to the grain surface in the pellets,
surface, diminishing inter-particle friction, and consequently affecting causing excessive plasticity and deformations. Moreover, the rise in the
force transmission between rolls and feed, resulting in an inferior pre­ shock temperature of green pellets could be attributed to the abundance
treatment. Fig. 5 illustrates that as the feed moisture in HPGR increased of hydrophilic groups in PTB. These groups hindered the evaporation of
from 9.0% to 10.5%, the drop number of green pellets initially rose to free water and the desorption of bound water during the drying process.
4.3 times/0.5 m, followed by a minor decline. Meanwhile, the shock In contrast, bentonite positively affected the compressive strength of
temperature of green pellets decreased from 423 ◦ C to 415 ◦ C due to green and dried pellets, which could be attributed to the robustly braced
heightened micro-particle presence and hindered water vapor diffusion fiber structure resulting from the inclusion of bentonite within the pel­
resulting from HPGR pretreatment. However, the compressive strength lets [30]. In summary, the incorporation of 2.0% or 1.0% composite

(a) 3.5 Drop number

15.5 455 (b) 5.0 Drop number
17.0 440
Compressive strength 450 Compressive strength 16.5
4.5 430
Compressive strength (N/P)

Compressive strength (N/P)

Drop number (times/0.5 m)

Drop number (times/0.5 m)

Shock temperature 15.0 Shock temperature

3.0
)

445 16.0
4.0 420
Shock temperature (

Shock temperature (

14.5
2.5 440 15.5
3.5 410
14.0 435
15.0
3.0 400
2.0 430
13.5 14.5
2.5 Minimum value 390
425
1.5 14.0
13.0 2.0 380
420
Blaine number:1726.34 cm /g 2 Blaine number: 1973.09 cm 2/g 13.5
1.0 12.5 415 1.5 370
1.6 1.8 2.0 2.2 1.6 1.8 2.0 2.2
Bentonite dosage (wt.%) Bentonite dosage (wt.%)

Fig. 4. Effect of bentonite ratios on the quality of green pellets with various Blaine numbers of the mixture: (a) Blaine number of 1726.34 cm2/g, (b) Blaine number
of 1973.09 cm2/g. (For interpretation of the references to color in this figure legend, the reader is referred to the Web version of this article.)

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Y. Ma et al. Journal of Materials Research and Technology 27 (2023) 6900–6911

(a) 4.5 Drop number

17.0 430 (b) 70

Dry compression strength (N/P)

Compressive strength

Compressive strength (N/P)

Drop number (times/0.5 m) Shock temperature 16.5
65

)
425

Shock temperature (
4.0 60
16.0
420 55
Minimum value
15.5
3.5 50
415
15.0
45

3.0 14.5 410 40

9.0 9.5 10.0 10.5 9.0 9.5 10.0 10.5
Moisture of feed in HPGR (wt.%) Moisture of feed in HPGR (wt.%)

Fig. 5. Effect of feed moisture in HPGR on the quality of green pellets: (a) Drop number, compressive strength, and shock temperature, (b) Dry compression strength.
(For interpretation of the references to color in this figure legend, the reader is referred to the Web version of this article.)

Table 4
Effect of PTB composite bentonite on the performances of green pellets.
Raw material ratio Bentonite ratio (wt. PTB ratio (wt. Drop number (times/ Compressive strength Shock temperature Dry compression strength
(wt.%) %) %) 0.5 m) (N/P) (◦ C) (N/P)

0 0.15 3.5 10.2 350 19.1

65A,35B 0.20 4.2 9.5 366 19.4
0.5 0.10 3.4 12.4 411 32.6
0.15 4.3 12.5 419 29.7
0.8 0.05 3.7 13.8 410 40.5
0.10 5.1 13.5 430 38.5
1.0 0.01 4.0 13.1 421 47.6
0.04 5.3 13.5 425 45.1
60A, 40B 1.0 0.01 3.8 13.9 420 48.5
1.0 0.04 4.8 13.6 423 43.2
55A, 45B 1.0 0.01 3.4 14.3 424 45.7
1.0 0.04 4.4 13.2 427 41.3

bentonite with 0.01% PTB yielded comparable pellet quality under higher capillary pressure, while the latter contributed to a higher drop
identical conditions. number of green pellets. Additionally, the viscosities of binder solutions
The potential of PTB in reducing bentonite dosage was further for the two green pellets were determined to be 4.05 mPa⋅s and 9.72
investigated using various mixing schemes. The results revealed a mPa⋅s, respectively, demonstrating the former experienced less viscous
noteworthy decrease in the drop number of the green pellets prepared as forces than the latter. It was evident that the combination of capillary
the proportion of hematite in the mixture increased. This decrease could force, viscous force, and porosity in green pellets resulted in comparable
be ascribed to the difficult ballability of concentrate B, along with var­ quality, even with a 1% difference in binder dosage.
iations in the strength of interaction between PTB and both magnetite
and hematite. 3.3. Drying performance of green pellets

3.2.4. Effect of PTB on the porosity, capillary radius, and solution viscosity 3.3.1. Effect of PTB on the drying rate of green pellets
in green pellets As mentioned earlier, configuration І exhibited a shock temperature
Table 5 compares the porosity and capillary radius of green pellets of 417 ◦ C, while configuration II reached a slightly higher temperature
with 2.0% bentonite (configuration І) to those with 1.0% bentonite and of 421 ◦ C. Consequently, subsequent drying experiments were carried
0.01% PTB (configuration II). The porosities of them were 17.16% and out at temperatures of 400 ◦ C or lower, and the results are shown in
24.87%, with corresponding capillary radii of 0.471 mm and 0.753 mm, Fig. 6. During the drying process, the dehydration rate of green pellets
respectively. Higher porosity enabled increased buffering through in­ increased rapidly with prolonged drying time until it reached a certain
ternal particle slip during the dropping of green pellets, while a larger value, after which it tended to stabilize for all types of pellets.
capillary radius decreased capillary force and particle interaction. As a Furthermore, pellets with the same binder exhibited a substantial in­
result, the former case subjected the inner particles of green pellets to crease in dehydration rate at higher drying temperatures. At a drying
temperature of 400 ◦ C, configurations І and II had average drying rates
of 0.296 g/s and 0.228 g/s, respectively. The maximum drying rates of
Table 5 these two types of pellets were 0.750 g/s and 0.500 g/s, respectively.
Porosity, capillary radius, and solution viscosity in green pellets with different Both the average and maximum drying rates of the former were faster
binder.
than those of the latter. The time to reach the maximum dehydration
Binder dosage (wt. Porosity Capillary radius The viscosity of 1% rate was ~180 s for the former and ~220 s for the latter, notably shorter
%) (%) (mm) solution (mPa⋅s)
for the former.
2.0 Bentonite 17.16 0.4713 4.05 This phenomenon can be attributed to the presence of PTB, which
1.0 Bentonite + 24.87 0.7532 9.72 effectively lowered the evaporation of inner water. Specifically, the
0.01 PTB
structure of PTB contains numerous polar and hydrophilic groups, such

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Y. Ma et al. Journal of Materials Research and Technology 27 (2023) 6900–6911

(a)100 (b)100

80 80
Dehydration rate (%)

Dehydration rate (%)

Binder: 2.0% Bentonite Binder: 1.0% Bentonite
60 60 +0.01% PTB
250
300 250
350 300
40 40 350
400
400
20 20

0 0
0 100 200 300 400 0 100 200 300 400
Drying time (s) Drying time (s)
(c) 0.8 (d)
100
0.7
Drying temperature: 400 80

Dehydration rate (%)

0.6
2.0% Bentonite
Drying rate (g/s)

0.5 1.0% Bentonite+0.01% PTB

60 Drying temperature: 400
0.4 2.0% Bentonite
1.0% Bentonite+0.01% PTB
0.3 40

0.2
20
0.1

0.0 0
0 50 100 150 200 250 300 0 50 100 150 200 250 300
Drying time (s) Drying time (s)

Fig. 6. (a, b) Effect of drying time on the dehydration rate of configurations І and II at different temperatures, (c) Variation of drying rate with drying time for
configurations І and II at 400 ◦ C, (d) Comparison of dehydration rate trends for configurations І and II at 400 ◦ C.

as –OH and –COOH, which bond to the particles surface through the
surface bonding, and the hydrophilicity of iron particles was also
improved due to the attachment of binder [1,31,32]. Consequently, the
desorption of hydroscopic water was decelerated, ultimately resulting in
a higher shock temperature.
3.3.2. Effect of PTB on the compressive strength and porosity of drying
pellets
The change in compressive strength during drying was a vital aspect
of the green pellet drying process. Notably, the compressive strength of
dried pellets showed a positive correlation with tensile strength [33].
Therefore, it was essential to investigate the compressive strength of
dried pellets to evaluate overall quality comprehensively. In this work,
we investigated changes in the compressive strength of green pellets and
the appearance of dried pellets with different binders during the drying
process, as shown in Fig. 7. The compressive strength of the pellets
increased slightly during the initial stage of drying at 400 ◦ C and
increased significantly after approximately 200 s. Overall, the
compressive strength of configuration II was lower than that of config­
uration І, particularly after 300 s of drying. After 380 s of drying, the
compressive strength of the former decreased, whereas the latter
continued to increase slowly. Despite significant differences in
compressive strength, there was only a minor distinction in their
appearance after complete drying. Moreover, the red coloration of
certain pellets indicated the oxidation of magnetite to hematite within
them.
The porosity and pore size distribution of configurations І and II were
further compared after thorough drying when the dehydration rate had
stabilized at 400 ◦ C. As depicted in Fig. 7, the porosity, average pore
size, and maximum pore size of the former were 27.31%, 0.669 μm, and
0.673 μm, while those of the latter were 29.27%, 0.775 μm, and 0.828
μm, respectively. The results caused by applying PTB could be revealed
from the changes of grain size composition because the long-chain PTB
with active functional groups could adhere to several or dozens of par­
ticles to form a large agglomeration.
3.4. Mechanisms of PTB to improve the quality of green pellets
3.4.1. FTIR analysis
Wetting and adsorption of the binder onto the surface of iron
concentrate particles are prerequisites for their bonding, and the binder
can be dissolved in the aqueous medium as a liquid bridge or fiber
structure attached to the surface of particles to facilitate bonding [34].
Since FTIR can convert the vibrational and stretching information of
chemical bonds in molecules into visualized wave numbers and ab­
sorption peaks of different morphologies, it can be used to verify
changes in functional groups on the iron concentrates surface before and
after binder adsorption. The FTIR spectra of magnetite after interaction
with different binders are presented in Fig. 8(a). As illustrated in Fig. 8
(a), the enhanced Si–O (1034 cm-1) and weakened Fe–O vibrational peak
(579 cm-1) of magnetite interacting with bentonite may be attributed to
the adsorption and reaction of Si oxides on Fe oxides [35]. In contrast to
bentonite, the O–H band vibration in magnetite significantly enhanced
and shifted to a higher wavenumber after reacting with PTB, indicating
strong adsorption of O–H in PTB onto the magnetite surface. The
decrease in intensity of the Si–O peak can be associated with the surface
complexation of Si–O by PTB molecules [36]. Furthermore, the
strengthening of –COOH stretching vibration (1467 cm-1) implies the

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Y. Ma et al. Journal of Materials Research and Technology 27 (2023) 6900–6911

Fig. 7. (a) Changes in compressive strength of pellets during drying, (b) The shape of dried pellets, (c, d) The porosity and pore size distribution of dried pellets.

(a) (b) Hematite+Bentonite+PTB H-O-H Si-O-Si

Magnetite+Bentonite+PTB 1467 1034 579
Hematite+PTB
Magnetite+PTB
Transmittance (%)

Transmittance (%)

Hematite+Bentonite
Magnetite+Bentonite
PTB
PTB

Bentonite 1639 Bentonite

H-O-H Si-O-Si
Magnetite Hematite

O-H O-H -COOH Si-O Fe-O O-H O-H -COOH Si-O

4000 3500 3000 2500 2000 1500 1000 500 4000 3500 3000 2500 2000 1500 1000 500
-1 -1
Wavenumber (cm ) Wavenumber (cm

Fig. 8. FTIR spectra of iron concentrates before and after reaction with binders: (a) Magnetite, (b) Hematite.

monodentate chelating of –COOH with Fe [37]. Where the peak in­
tensity of O–H, –COOH, and Fe–O located at ~2934, ~1467, and ~579
cm-1 weakened after the reaction of magnetite with bentonite and PTB,
indicating that Si oxides in bentonite adsorbed on Fe oxides of magne­
tite, and PTB molecules adsorbed onto the surfaces of both magnetite
and bentonite through O–H hydrogen bond and surface complexation of
–COOH.
As illustrated in Fig. 8(b), there were no noteworthy alterations in
the peak pattern and intensity of FTIR spectra before and after the
interaction involving hematite, bentonite, and PTB. This indicates a
relatively weak interaction among these three components. Therefore,
the subsequent investigation was focused on the bonding mechanism
between PTB and the iron surface of the iron concentrate.

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Y. Ma et al.
3.4.2. XPS analysis
To give insight into the PTB adsorption pathway, XPS was further
conducted to investigate the elemental composition, valence, and
binding forms of the iron concentrate surface before and after its reac­
tion with PTB. As depicted in Fig. S1, the survey spectra of unreacted
magnetite revealed the presence of Si, C, O, and Fe at binding energies
~102.5, ~285.4, ~531.2, and ~711.5 eV, respectively. In the high-
resolution C 1s spectra, three peaks were observed at ~284.8, ~285.9,
and ~288.9 eV, corresponding to C–C/C–H, C–O/C–N, and C=O,
respectively [38]. Simultaneously, the O 1s spectra were deconvoluted
into three peaks at ~530.0 eV (M− O), ~530.9 eV (O–H), and ~532.3 eV
(C–O). The fitting of the photoelectron peaks (Fig. 9(d)) at
~710.4/~723.5 eV (Fe 2p3/2) and ~712.5/~725.6 eV (Fe 2p1/2) indi­
cated of Fe(II) and Fe(III) [39]. After the reaction, the peaks in survey
spectra of C 1s and O 1s might originate from the oxide layer or C and O
associated with PTB. Additionally, the content of C–C/C–H decreased,
while that of C–O and C=O in the C 1s spectra increased, potentially due
to coordination between oxygen groups and Fe [40]. Besides, the pro­
portion of C–O and O–H in the O 1s spectra increased (consistent with
the C 1s spectral fitting), and the peak corresponding to –COOH
(~533.9 eV) appeared, demonstrating the involvement of hydroxyl and
carboxyl groups in adsorption, which may be attributed to the oxygen
atoms providing lone pairs of electrons to iron, resulting in a decrease in
surrounding electron density [41]. Notably, the relative area ratio of Fe
(II)/Fe(III) remained basically unchanged before and after adsorption,
suggesting that the no redox reaction occurred during PTB adsorption on
the magnetite surface.
Fig. S2 illustrates the survey spectra of hematite before and after
adsorption. The peaks at ~102.5, ~285.4, ~531.2, and ~711.5 eV
could be ascribed to Si, C, O, and Fe, respectively. As mentioned above,
the relative proportion of Fe(II)/Fe(III) remained unchanged after the
reaction, indicating the absence of a redox process. Furthermore, the
proportion of C–O/C–N and C=O increased, which might be due to the
coordination with Fe [36]. However, these changes were poorly re­
flected in the FTIR spectra of hematite after adsorption, demonstrating a
relatively weak PTB adsorption on the hematite surface. Therefore, It
Fig. 9. XPS spectra of iron concentrates before and after reaction with PTB: (a–c) C 1s, O 1s, Fe 2p spectra of magnetite; (d–f) C 1s, O 1s, Fe 2p spectra of hematite.
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Journal of Materials Research and Technology 27 (2023) 6900–6911
can be inferred that PTB was adsorbed on the magnetite surface through
hydroxyl, carboxyl, and other oxygen groups by hydrogen bond, surface
complexation and coordination. The XPS analysis was also in agreement
with the results of FTIR analyses.
Differences in PTB adsorption onto magnetite and hematite surfaces
might be related to the characteristics of the solution environment. It is
important to note that the reaction between iron concentrates and PTB
occurred in a solution with a pH of 10.0 at 25 ◦ C, with the solution pH
being governed by the intrinsic properties of PTB. In solution systems,
magnetite particles are more easily hydrated, leading to complete sur­
face coverage by Fe–OH groups. The Fe–OH sites on the surface can
interact with OH- ions in alkaline solutions, leading to the development
of negative (Fe–O-) charges through protolytic reactions [17,42]:
Fe − OH + OH− ⇔ Fe − O− + H2 O (3)
-
Therefore, the presence of Fe–O and –OH groups on the magnetite
surface facilitated chemical interaction with the active groups in PTB,
resulting in adsorption.
3.4.3. SEM-EDS analysis
For the observation of adsorption behavior more clearly for the iron
concentrates with PTB, SEM-EDS analysis was conducted to investigate
sample morphology. As depicted in Fig. 10(a), the surface of magnetite
particles appeared relatively smooth before adsorption, with tiny par­
ticles (1–2 μm) dispersed among larger ones (~10 μm), but there was no
obvious bridging observed. EDS results indicated the main elements
were Fe, O, and Si. After the reaction, a fibrous structure was observed
(Fig. 10(b)), indicating the bridging of magnetite particles with varying
morphologies by PTB. EDS analyses revealed that the primary elements
in this fibrous bridge were O, Fe, C, and Si, particularly with a significant
increase in C content (8.42%) compared to before adsorption. This in­
crease affirmed that the inter-particle bridges were primarily composed
of the fibrous molecular structure formed by PTB dissolution. However,
the uneven distribution of the fiber structure suggested that PTB and
magnetite were not homogeneous adsorption, possibly due to the high
viscosity characteristics of PTB molecules, which significantly increased
Y. Ma et al.
Fig. 10. SEM images and EDS results of iron concentrates before and after adsorption PTB: (a, b) Before and after of magnetite, (c, d) Before and after of hematite.
upon dissolution in water. Moreover, their adsorption on the surface of
magnetite particles was influenced by factors such as surface polarity,
pore structure, and specific surface area [36].
The initial SEM image of hematite (Fig. 10(c)) revealed angular
particles and EDS results identified the main elements as O, Fe, Si, Al,
and Ca. Upon interaction with PTB, the surface of hematite particles
displayed a similar fibrous structure, but EDS analysis indicated no
substantial alteration in elemental C. To quantify the variation in
elemental carbon (C) content on the iron concentrates surface before
and after PTB adsorption, carbon and sulfur analyzers were utilized,
with results detailed in Table S1. For magnetite, the C content increased
from 0.143% to 0.279% post-PTB adsorption, whereas for hematite, it
changed from 0.086% to 0.111%. These findings corroborate the pre­
dominant adsorption of PTB on magnetite surfaces, aligning with FTIR
and XPS analysis results.
3.4.4. Potential mechanisms
In conclusion, the mechanisms illustrating how PTB composite
bentonite enhances the quality of green pellets are presented in Fig. 11.
During the pelletizing, trace amounts of PTB adsorbed onto the surface
of iron concentrates (mainly magnetite) through hydrogen bonding,
monodentate chelating, coordination, electrostatic repulsion, and other
Fig. 11. Mechanism diagram of PTB in green pellet. (For interpretation of the references to color in this figure legend, the reader is referred to the Web version of
this article.)
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Journal of Materials Research and Technology 27 (2023) 6900–6911
mechanisms. It also adsorbed onto the surface of bentonite through
surface complexation, and subsequently dissolved into a fiber structure
that bridged the particles together in green pellets. Simultaneously, a
mass of bentonite plates was coated on the surface of iron ore particles,
which provided robust support for the green pellets under the action of
hydration. Consequently, the incorporation of trace PTB into bentonite
significantly enhanced the drop number and compressive strength of
green pellets. During the drying process, the hydrophilic groups in PTB
markedly increased the water-holding capacity of green pellets, result­
ing in a noticeable reduction in the dehydration rate and a substantial
increase in the shock temperature of green pellets.
4. Conclusions
In this study, we investigated the action performance and intrinsic
mechanism of polymer-type binder (PTB) aimed at reducing bentonite
consumption in pelletizing. PTB was abundant in functional groups (e.
g., –OH, –COOH, –C=C-) and exhibited high viscosity properties, mak­
ing it highly efficient. The addition of just 0.01% PTB reduced the
bentonite ratio by 1% during the pelletizing process, resulting in the
preparation of high-quality green pellets, even when using under­
performing pelletizing feeds. Furthermore, the inclusion of PTB
Y. Ma et al.
significantly increased the drop number and shock temperature of green
pellets. FTIR, XPS and SEM-EDS analyses demonstrated that this
improvement was mainly attributed to PTB’s adsorption on the surfaces
of magnetite and bentonite through hydrogen bonding, electrostatic
repulsion, monodentate chelating, surface complexation, etc., facili­
tating the bridging of discrete particles with different sizes. Moreover,
PTB dramatically enhanced the water-holding capacity of green pellets,
and the reduced dehydration rate during the drying process played a
crucial role in elevating the shock temperature of green pellets. Overall,
this research provided valuable technical insights into reducing
bentonite usage in the pelletizing process of the iron and steel industry,
thereby contributing to improved quality and reduced carbon emissions.
Data availability
No data was used for the research described in the article.
CRediT authorship contribution statement
Yonghe Ma: Investigation,Writing – original draft.Qian Li:
Conceptualization,Writing – review & editing.Yan Zhang: Supervision.
Yongbin Yang: Writing – review & editing.Yinhua Tang: Writing –
review & editing.Tao Jiang: Writing – review & editing.
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.
Acknowledgments
We gratefully acknowledge the support by the National Key Research
and Development Program of China (No. 2023YFC2907801), the
Fundamental Research Funds for the Central Universities of Central
South University (No. 202044023) and the Hunan Provincial Natural
Science Foundation of China (No. 2023JJ40760).
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.jmrt.2023.11.134.
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