Powder Technology 319 (2017) 1–11

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Powder Technology

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

Review

Recent advances in effective collectors for enhancing the flotation of low

rank/oxidized coals
Baofeng Wen a, Wencheng Xia a,⁎, Jovica M. Sokolovic b
a
Key Laboratory of Coal Processing and Efficient Utilization of the Ministry of Education, School of Chemical Engineering and Technology, China University of Mining and Technology,
Xuzhou 221116, Jiangsu, China
b
University of Belgrade, Technical Faculty in Bor, Vojske Jugoslavije 12, 19210 Bor, Serbia

a r t i c l e i n f o a b s t r a c t

Article history: Coal plays an important role in energy supply. However, low rank/oxidized coals are difficult to float with the
Received 7 November 2016 common oily collectors, and hence effective collectors are urgently needed to be found or created. The
Received in revised form 4 June 2017 difficult-to-float reason of low rank/oxidized coals primarily includes two aspects, i.e. abundant oxygen-
Accepted 14 June 2017
containing groups on coal surface and porous surface of coal particle. The common oily collectors are difficult
Available online 15 June 2017
to adsorb on hydrophilic sites on low rank/oxidized coals surface and a porous structure of coal surface
Keywords:
needs large consumption of collectors. This review is to highlight recent advances in the effective collectors for
Low rank coal enhancing the flotation of low rank/oxidized coals, especially an overview of effective collectors proposed
Oxidized coal in the past decade. The effective collectors are achieved through the emulsion of common oily collectors, the
Collectors mixture of several collectors/surfactants, the special collectors and bio-collectors. Throughout this review,
Mechanism the mechanism of the effective collectors enhancing the flotation of low rank/oxidized coals is discussed and
Flotation the development directions of effective collectors in the future are also recommended.
© 2017 Elsevier B.V. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
2. Characters of low rank/oxidized coals surface . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
3. Common oily collectors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
4. Effective and special collectors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
4.1. Emulsion and mixture of common oily collectors and others . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
4.2. Special collectors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
5. Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10

1. Introduction
As the demand for energy growth, coal plays an important role in
energy supply and hence fine coals are urgently needed to be effectively
recycled. Froth flotation is usually considered to be the most effectual
method to upgrade the fine coal (b 0.5 mm) [1]. On a worldwide basis,
there are from 0 to 40% of the coal which are normally upgraded by flo-
tation [2]. In the conventional coal flotation, the coal usually has natural
hydrophobic surface while the mineral has natural hydrophilic surface.
⁎ Corresponding author.
E-mail addresses: xiawencheng@cumt.edu.cn, w.xia.cumt@gmail.com (W. Xia).
Exactly, flotation uses this difference in the surface properties of coal
and mineral to separate the coal by bubbles from the minerals in the
flotation pulp. Most of the coal enters into the froth product becoming
the concentrate, while most of the mineral stays in the pulp becoming
the tailings. In the froth flotation, a few coals cannot become the
concentrate, which causes the loss in the combustible matter recovery
as well as clean coal yield. However, a few minerals can also enter into
the froth product, namely, the entrainment of high-ash minerals [3,4].
The coal is made up of the organic compositions, such as aliphatic
hydrocarbons and aromatic series [5]. In contrast, the mineral in raw
coal primarily consists of clays, such as carbonate minerals, gypsum,
quartz, and pyrite. These minerals in the coal are normally hydrophilic.
In a word, the coal is normally easy to float and separate from the

http://dx.doi.org/10.1016/j.powtec.2017.06.030
0032-5910/© 2017 Elsevier B.V. All rights reserved.
2 B. Wen et al. / Powder Technology 319 (2017) 1–11
minerals based on the difference in natural hydrophobicity between the
coal and the minerals.
However, there are lots of low rank coals which are difficult to float
with typical oily collectors in moderate additions [6–10]. A delegate
for low rank coals is lignite. Lignite is generally hydrophilic due to the
presence of a large amount of oxygen-containing groups. Meanwhile,
the high-rank coal is easy to be oxidized in the air. The oxidation pro-
cesses result in the formation of oxygen-containing functional groups
on the high-rank coal surface, which reduces the hydrophobicity of
the high-rank coal surface [11,12].
In other words, low rank and oxidized coals are similar in the surface
properties and the role of collectors in the flotation of low rank coal is
also similar to that in the flotation of oxidized coal. This review is to
highlight recent advances in the effective collectors for enhancing the
flotation of low rank/oxidized coals. The mechanism of the effective
collectors enhancing the flotation of low rank and oxidized coals will
be also discussed. This review does not focus on the reverse flotation
collectors of low rank/oxidized coals because an overview of reverse flo-
tation process for coal has been published [13].
2. Characters of low rank/oxidized coals surface
Low rank coals include peat, lignite and some sub-bituminous coals.
All of these coals are characterized by low metamorphic degree. Coal
is formed from plant materials after the long periods of compression
and hardening. During the periods of the formation of coal, the oxygen
content is reduced while the carbon content is increased. The carbon
content/oxygen content ratio decreases with the increase of coal
rank. The carbon content of anthracite coal reaches the highest value
while the oxygen content is the lowest compared with other coals
at different ranks, i.e. lignite, sub-bituminous coals and bituminous
coals. The oxygen exists in the coal as the primary forms of oxygen-
containing functional groups. Carboxyl, phenolic and carbonyl are the
primary oxygen-containing functional groups in low rank coals. These
oxygen-containing functional groups can be bonded with water mole-
cules by hydrogen bonding, which reduces the hydrophobicity of low
rank coal surface. Therefore, low rank coals are difficult to float with
common oily collectors. The common oily collector cannot easily spread
on the surface of low rank coals. According to this situation, the collec-
tors containing the oxygenated functional groups have an important
role on the flotation of low rank coals [14,15]. In addition, the surface
topography of low rank coal is rough and porous. When low rank coal
is pre-wetted in the flotation pulp, a thick water film will cover its
surface [16]. The conventional oily collector is prevented to effectively
adsorb on low rank coal surface. The porous surface properties of low
rank coals also increase the consumption of collectors and flotation
costs [17–19].
At the same time, the flotation of oxidized coal is a key issue. The two
types of coal, i.e. bituminous and anthracite coals are usually easy to
float with the common oil collectors due to their high natural hydropho-
bicities. However, they can be oxidized in the air. The oxidation reduces
the hydrophobic sites on the coal surface. The oxidation reaction also re-
sults in the formation of oxygenated functional groups on the coal sur-
face and hence the natural hydrophobicity of the coal will be reduced
after the oxidation. The oxidation of the coal surface makes the coal
difficult to float using common oily collectors [20,21]. Coal oxidation in-
cludes three major aspects, namely, the adsorption of oxygen on coal
surface, the release of reaction products (like H2O, CO2 and CO), and
the release of heat [22–27]. Sometimes, the release of heat may cause
the coal to be oxidized to a further extent. For the mild oxidation, the
oxidation only occurs on the coal surface and the surface properties of
coal can be significantly changed. However, for the heavy oxidation,
the oxidation can occur in the inner of coal particles and hence the
whole coal is oxidized [28,29]. After the oxidation, the surface proper-
ties of oxidized coal are similar to those of low rank coal. As shown in
Fig. 1, XPS and SEM pictures of lignite and oxidized coal surface are
similar [30,31]. Both lignite and oxidized coal surface have abundant
oxygen-containing groups and porous structure.
The grinding pretreatment has been widely used in the recovery of
the hydrophobicity of oxidized coal. The oxidized layer on coal surface
can be removed and the fresh and hydrophobic surfaces are exposed.
After the grinding or attrition pretreatments, the surface hydrophilicity
of the oxidized coals is generally reduced [32–37]. However, the heavy
oxidized coal is difficult to obtain a good hydrophobicity through the
grinding or attrition pretreatments [28]. In this case, the effective collec-
tor is the only way to float them effectively.
3. Common oily collectors
In coal flotation industry, the common oily collectors are fuel oils,
such as kerosene and diesel oil. In the experimental study, the common
oily collectors are dodecane and hexadecane. The oily collectors primar-
ily consist of carbon and hydrogen elements. In some cases, the com-
mon oily collectors are named as hydrocarbon oils. The carbon and
hydrogen elements usually exist as the forms of\\CH3,\\CH2,\\CH in
the oily collectors. The groups,\\CH3,\\CH2 and\\CH are hydrophobic
and can spread easily on the hydrophobic sites on the high-rank coal
surface [38]. While the coal is low rank or the coal is oxidized, there
are only a few hydrophobic sites on the coal surface. The oily collectors
are difficult to have an effective spread or adsorption on the low rank/
oxidized coal surface [16,39,40]. Therefore, the hydrophobicity or
floatability can be hardly enhanced by the oily collectors.
In addition, the dosage of oily collectors is also very high in order to
create a high reagent concentration for the effective spread or adsorp-
tion of the oily collectors on the coal surface. Especially for low rank
and oxidized coals, the high reagent concentration is somewhat useful
for obtaining the high flotation recovery [7]. Therefore, the reagent
dosage in the flotation of low rank/oxidized coals is usually much
higher than the reagent dosage in the flotation of bituminous and an-
thracite coals. Many coal preparation plants usually adopt this method
(increasing collector dose) to enhance the flotation recovery of low
rank and oxidized coals [14]. However, a high reagent dosage can also
somewhat decrease the selectivity, which increases the ash content of
clean coal because the hydrophobicity of some ash minerals will be
also enhanced at a high collector dosage condition [4]. Furthermore, a
high dose of oily collectors in coal flotation is not economic. Therefore,
it is urgent that the effective collectors should be found to enhance
the flotation of low rank and oxidized coals.
4. Effective and special collectors
4.1. Emulsion and mixture of common oily collectors and others
Usually, the common oily collectors spread on the coal surface as the
form of small oil drops. The oily collectors, such as kerosene and diesel
oil are broken into amounts of small oil drops by the impeller or stirring
devices. The diameter of small oil drops is usually several microns. The
hydrophobicity of coal surface can be enhanced by the adsorption
of the small oil drops on its surface. In recent years, the emulsion tech-
nology for the effective distribution of the oily collectors is widely ap-
plied in the conditioning and flotation processes. Benefiting from this
emulsion technology, the collector dosage is decreased as well as the
distribution condition is improved [41]. Ahmed and Drzymala [42] com-
pared the flotation behavior of oxidized coal by the direct contact with
pure (anhydrous) flotation reagent or microemulsion, and they found
that mixing dry oxidized coal with microemulsion droplets achieved
higher clean coal yield.
Shen et al. [43] used fatty acids emulsions in the reverse flotation
of Pingsuo gas coal fines and found the emulsions not only reduced
the clean coal ash content but also save the reagents consumption.
They used two types of emulsions obtained from oleic acid and do-
decanoic acid emulsified by dodecylamine hydrochloride (DDA-HCL),
 B. Wen et al. / Powder Technology 319 (2017) 1–11 3

(a) XPS and SEM pictures of lignite [30]

(b) XPS and SEM pictures of oxidized coal [31]

Fig. 1. XPS and SEM pictures of lignite and oxidized coal surface.

respectively. They claimed that the droplet sizes of the two emulsions
were much smaller than those of the pure oleic acid and dodecanoic
acid. Meanwhile, they proposed a probable interaction mechanism be-
tween fine gangue mineral and the emulsions or DDA-HCL. As shown
in Fig. 2, DDA-HCL hydrocarbon chain might be inserted into the inside
of oil droplets, while the polar head was at oil–water interface towards
the water phase. The use of DDA-HCL changed the zeta potential of fatty
acid value from negative to positive. Therefore, a strong electrostatic at-
traction between minerals particles and the emulsion droplets could be
built which enhanced the adhesion of the emulsion droplets on mineral

Fig. 2. Schematic representation of probable interaction mechanism between gangue minerals and (a) dodecylamine hydrochloride and (b) fatty acids emulsions [43].
4 B. Wen et al. / Powder Technology 319 (2017) 1–11
surface. In addition, the adsorption of hydrophobic fatty acid on gangue
mineral surface increased the hydrophobicity of the gangue particles
which were easy to float into the froth and hence the clean coal ash
was reduced.
In another study, Laskowski and Yu [44] used the emulsification of
kerosene (in the presence of surfactants) in the oil agglomeration of
oxidized bituminous coal from Fording mine in British Columbia. They
also found that the surfactants not only reduced the size of the kerosene
droplets but also decreased the consumption of kerosene required in
the oil agglomerate processes. They claimed that the surfactants used
in the emulsification of kerosene changed the electro-kinetic properties
of the oil droplets and enhanced the particle–oil droplet interaction. The
cationic oil emulsions were effective for the oil agglomerate of oxidized
coals because their surface electro-kinetic potentials were negative
values.
Xie et al. [45] used a new emulsified flotation reagent for enhancing
1/3 coking coal flotation. The new emulsified flotation reagent was pre-
pared by 3% flotation promoter (synthesized with natural cottonseed oil
and industrial by-products), 27% diesel oil and 70% water. They claimed
that the coal treated by this promoter had an increase in the surface
hydrophobicity because the chemisorption occurred between the
promoter and the coal surface. The spreading of hydrocarbon oil on
the coal surface could be sped up by the usage of this new emulsified
flotation reagent. As a result, the adsorption of emulsified oil on the
coal particle surface was improved and the flotation rate was also en-
hanced. Zhu et al. [46] also used this emulsified flotation reagent for
the flotation of Qianjiaying and Huaixiao coal samples. The emulsified
flotation reagent showed the excellent performance, good stability
and high selectivity compared with diesel. However, the dosage of
emulsified flotation reagent in coal flotation was lower than diesel.
Saleh [47] also proved that the fuel oil collector after the emulsification
by pine oil could increase the coal flotation recovery/rate because the
oil/water interfacial tension and energy required to spread fuel oil col-
lector on the coal surface were significantly reduced. The coal surface
hydrophobicity would be greatly enhanced and the required collectors
could be also saved. The emulsification technology should be adapted
to optimize and maximize the flotation recovery of coal, especially for
low rank and oxidized coals.
Mixing the common oily collectors with the surfactants or other
hydrocarbon oils to form an effective collector is useful for the en-
hancement in the flotation of low rank and oxidized coals. The usage
of various surfactants could improve the dispersion and adsorption of
oil collectors on the coal particles [48–51]. In other studies, the mixture
of frothers also played an important role in coal flotation [52,53]. Using
non-ionic surfactants as collectors has been proved to be effective in
improving the surface hydrophobicity of oxidized and low rank coals
[14,54]. Celik [55] found the block co-polymers (pluronic L-64 and
10R-8) was useful for the increase of flotation recovery of lignite. The
mixture of methyl isobutyl carbinol (MIBC) with poly(ethylene glycol)
tert-octylphenyl ether (Triton X-100) or sodium dodecyl sulfate (SDS)
could increase the solid recovery, and the mechanism of the mixture
enhancing coal flotation was considered that MIBC could act as two
roles such as collecting role and frothing role because MIBC could se-
lectively adsorb on solids and hence the solid recovery [56]. Erol et al.
[57] pointed out that the mixture of Triton X-100 with MIBC used as
flotation reagent could improve the ash rejection. In another study,
Kelebek et al. [58] claimed that the significance of dodecylamine as a
collector was greater than that of kerosene and pH value also played
a significant role in the interactions between dodecylamine and coal
surface.
Wen and Sun [59] investigated the flotation of oxidized coal using a
composite mixture of fuel oil no. 2 and fuel oil no. 6 in a ratio of 4:1 and
found the mixture was effective for floating the oxidized coal. The oil
droplets of the mixture were found to have a higher positive charge be-
cause fuel oil no. 6 contained some polycyclic structures, such as amine,
sulfur, salts of nickel and vanadium. The polycyclic structures could be
easily bonded with the oxygen-containing functional groups and
hence enhance the surface hydrophobicity of the oxidized coal. Temel
and Majumder [60] also proved that the mixture of 80% kerosene and
20% fuel oil could improve the flotation recovery of Malatya-Arguvan
lignite. Compared with the sodium oleate and Aero 3477, the combusti-
ble matter yield using 80% kerosene and 20% fuel oil mixture was higher
than that using sodium oleate or Aero 3477. Qu et al. [19] studied the
mixture of Nalco 9858 and diesel oil as a collector to enhance the flota-
tion of Shendong low rank coal. The low rank coal floatability could
be greatly improved by the synergism of the nonionic surfactant and
mixed collector.
Jena et al. [61] claimed the black oil, a long-chain carbon atoms
reagent, could improve the floatability of oxidized coal of Talcher coal
field in India. They used a mixture of black oil and kerosene oil to float
the oxidized coal effectively. The black oil contained a more complex
mixture of C\\H/\\CHO/OH/COOH groups than kerosene oil. The black
oil might act as a promoter for the surface modification of oxidized
coal because the black oil could be easily bonded with the oxygen-
containing functional groups on the oxidized coal surface. As a result,
the yield of the froth product increased with the increasing collector
dosage but without significant changes in the concentrate ash content
as shown in Fig. 3.
Vamvuka and Agridiotis [62] pointed out both the combustible
matter recovery and concentrate ash content could be improved a
little using the kerosene oil as solo collectors during the flotation of
lignite from the Ptolemais–Amynteon Lignite Centre in North Greece.
However, the flotation performance of lignite would be greatly en-
hanced using a combination of kerosene and dodecylamine as flotation
reagents. In addition, the concentrate ash could be reduced using
dodecylamine as a solo collector. They also compared the effects of sur-
factant type on the flotation behavior of lignite at neutral pH value. Two
cationic surfactants, dodecylamine and Myristil–Trimethyl Ammonium
Bromide (TTAB), an anionic surfactant, sodium dodecyl sulfate (SDS)
and a non-ionic surfactant, 2-ethyl hexanol were compared. It was
found that the two cationic surfactants could be distinguished from
the others by having a much better selectivity, and then anionic surfac-
tant, non-ionic surfactant. As shown in Fig. 4, the ζ potential measure-
ments explained that the addition of surfactants could change the ζ
potential of lignite surface from negative to positive below pH = 8.5.
In addition, the pH value was considered to have an important role in
the adsorption of the surfactants onto the coal surface. By using the
Fig. 3. Effect of kerosene oil dosage on oxidized coal flotation combined with black oil
(0.5 ml/kg) as collector [61].
 B. Wen et al. / Powder Technology 319 (2017) 1–11
Fig. 4. Influence of surfactant type on variations of the electrokinetic potential of the lignite
as a function of pH (frother: 0.4 g/kg coal MIBC; pulp density: 15%) [62].
combination of surfactants and kerosene oil, the floatability of lignite
could be significantly enhanced and hence the effective flotation recov-
ery of lignite was achieved.
Xia et al. [63] used a mixture of dodecane and 4-dodecylphenol
(DDP) as the effective collector to improve the flotation of Inner
Mongolia lignite. They compared the flotation performance of lignite
using the mixture and DDP or dodecane. The clean coal yield using the
mixture was much higher than that using dodecane or DDP solely
while the clean coal ash using the mixture was lower than that using
dodecane or DDP solely. FTIR measurement was used to indicate the
mechanism of the mixture as collector enhancing lignite flotation.
As shown in Fig. 5, the peaks for hydrophobic groups in lignite were
enhanced after the conditioning with the mixture while the peak at
3384 cm−1 for \\OH was weakened. The hydrophobic groups were
enhanced while the hydrophilic groups were weakened as the mixture
was used as the collector. While the mixture of DDP and dodecane was
Fig. 5. FTIR spectrums of lignite before and after conditioning with collectors, A—original lignite, B—lignite conditioned with DDP, C—lignite conditioned with dodecane, D—lignite
conditioned with the mixture of DDP and dodecane [63].
5
used as the collector, the dodecane primarily covered the hydrophobic
sites on the lignite surface and the DDP primarily covered the hydro-
philic sites on the lignite surface. Therefore, the surface hydrophobicity
of lignite was improved after the conditioning with this mixture.
The surfactants are also used as pretreatment reagents for the flota-
tion of low rank coal. Ni et al. [64] pre-conditioned long flame coal with
the surfactant, polyoxyethylene sorbitan monostearate (Tween 60), and
then conditioned coal with the oily collector to improve the flotation
performance. They claimed that the contact angle of coal conditioned
with Tween 60 was higher than that of raw coal, which indicated the
surface hydrophobicity of coal was increased by Tween 60. Zhang
and Tang [30] also used sorbitan monooleate to pre-treat lignite and
obtained an improved flotation recovery.
4.2. Special collectors
Jia et al. [15] used THF esters [C4H7O\\CH2\\OOC\\R] to successfully
improve the floatability of low rank/oxidized coals. This type of collec-
tors containing a benzene ring owned a better collecting ability of
oxidized sites on coal surface compared with the dodecane. The hydro-
gen bonding of oxygen contained groups with coal surface in the collec-
tors was stronger than the van der Waal interaction of aliphatic chains
with carbonaceous portions of coal surface. The oxygen-containing
functional groups and the benzene ring in this type of collectors were
effective for the collection of low rank coals. The adsorption of the
THF series of collectors onto the coal surface could be explained by
the mechanisms as shown in Fig. 6: hydrogen bonding of oxygen
atoms with the oxygenated surface sites on the coal; hydrophobic
bonding of the aliphatic hydrocarbon chain with the hydrophobic
sites; π-bonding of the benzene ring on the hydrocarbon chain of the
collector with aromatic sites of coal surface. Introducing the benzene
ring into the collector could increase the collecting ability by a strong
π bonding between benzene ring and coal aromatic structure [65].
A combination of hydrophobic aliphatic hydrocarbon chain along with
aromatic compounds and hydrophilic groups could be effective as a
collector for oxidized coals [2,66,67].
Sis et al. [68,69] investigated the comparison of flotation of low rank
coal from Zonguldak Coal Washery in Turkey using kerosene, pine
oil, tall oil as the collector. The tall oil considered as ionic surfactant
6 B. Wen et al. / Powder Technology 319 (2017) 1–11
Fig. 6. Schematic representation of interaction between surfactant molecules and
coal surface, showing A as polar head and B as hydrocarbon chain, the affinity of the
individual functional group of a reagent for the coal surface is represented as α [15].
Fig. 7. Effect of collector (oil) amount and type on combustible matter recovery, ash rejection and efficiency index [72].
contained N40% of oleic acid. The ionic collectors had the significant ad-
vantages in reducing the concentrate ash content while kerosene and
pine oil could not obtain concentrate ash below 21–22%. The ionic col-
lectors were proved to be dispersed better than kerosene and hence de-
creased the entrapment of ash forming matter within the agglomerates.
Tall oil could help to reduce the surface tension of slurry which further
enhanced the bubble surface area inside the flotation cell. The mixture
of fatty acids could react with the oxygen groups on coal surface and
hence the floatability of oxidized coal could be increased resulting in
higher combustible matter recovery [70].
Chaudhuri et al. [71] created an improved collector (a particular coal
tar distillate fraction) derived from coal tar to improve the flotation re-
covery of low-volatile medium ash clean coal fines. Compared with
using the diesel or the dodecane as collectors, the clean coal yield
using the improved collector was about 83% which is much higher
than clean coal yield of 71.4% using the diesel and clean coal yield of
66.7% using the dodecane.
Sonmez and Cebeci [72] compared the flotation of Ukraine coal
using classic oils (kerosene, diesel-oil and fuel-oil) and lubricating oils
(spindle oil, bright stock and heavy neutral). As shown in Fig. 7, the flo-
tation results indicated that the combustible matter recovery using
bright stock was higher while the ash rejection was lower. They claimed
that the higher combustible recoveries with lower ash rejection using
bright stock were attributed to the non-selective adsorption of bright
stock on the organic materials and mineral matters. But for the effi-
ciency index values, the efficiency index using bright stock was rela-
tively higher, which indicated the bright stock should still have a good
selectivity. The mechanism of the adsorption of bright stock on coal sur-
face needs more fundamental analysis.
Vegetable oil has been found to be an effective collector for coal flo-
tation. Alonso et al. [73] found olive oil along with soybean oil could pro-
vide a substantial increase in the combustible matter recovery for low
rank coals. Meanwhile, researchers found vegetable oils were effective
for oil agglomerating of coal fines by the interactions occurring between
vegetable oils and coal surface through hydrogen bonding [74–76].
 B. Wen et al. / Powder Technology 319 (2017) 1–11
Fig. 8. FTIR spectrum of biodiesel (up) and diesel (down) [80].
Recently, researchers proposed that bio-oils could be considered as
alternative collectors for coal flotation [77–80]. These bio-oils were
obtained from vegetable oil and waste cooking oil. By doing this, the
problems of environmental pollution by waste cooking oil could be
solved and an alleviate coal collector was created [81,82]. Yang et al.
[83] compared the flotation of Huangling coal using kerosene, diesel,
drainage oil, and emulsified drainage oil as collectors, respectively.
They obtained the best recovery using emulsified drainage oil as collec-
tor while the yield of clean coal was 88.67% at the ash content of 8.63%.
In another study, Fecko et al. [84] obtained a new collector from the
pyrolysis products of waste plastics, tires and rubber. They combined
this collector with classical collector Montanol 551 to produce suitable
collectors for the flotation of black coal from Lazy Mine in Poland. In
addition, the flotation of this black coal was achieved using the mixture
of brown coal pyrolytic oils and Montanol 800 [85].
Xia et al. [80] used biodiesel to improve the flotation of Taixi
oxidized coal and found the biodiesel contained more abundant unsat-
urated fatty acids than the conventional diesel as shown in Fig. 8. They
claimed the biodiesel could be bonded with the oxygen contained
groups on coal surface through the weak hydrogen bonding.
The oxygen contained groups in the collectors are very important in
the effective adsorption on the surface of low rank/oxidized coals. In
other words, introducing the oxygen contained groups into the conven-
tional oily collectors is considered as a feasible way to the enhancement
in the flotation of low rank/oxidized coals. Even though the surfactants
are good at improving the flotation of low rank coal and somewhat can
be used as the collectors in low rank coal flotation. The oily collectors
are still essential for coal flotation because the surfactants may be
non-selective [18,30]. Therefore, a method to oxidize the conventional
Fig. 9. Comparison of flotation of oxidized coal using dodecane and oxidized diesel oil as collectors before and after grinding pretreatment [86].
7
oily collectors into oxygenated collectors is proposed. Xia and Yang
[86] compared the flotation performance of Taixi oxidized coal using
dodecane and oxidized diesel oil as the collectors, respectively. They
also applied the grinding pretreatments to reduce the oxidized coal par-
ticle size. As shown in Fig. 9, the oxidized diesel oil not only increased
the flotation recovery but also reduced the concentrate ash content.
Especially, the b 0.074 mm size fraction was greatly enhanced. Conse-
quently, oxidized coal particles with smaller size were more floatable
than coarse coal particles [32,86–88]. However, the mechanism of
why fine oxidized coal particles were more floatable than coarse parti-
cles needs more attention.
Recently, Xing et al. [89] used an oxygenated polar compound collec-
tor to enhance (named CC in their paper) the flotation of oxidized coal
and obtained excellent flotation results using the CC as the collector.
As shown in Fig. 10, the CC had more polar hydrophilic groups such as
peaks at 3424 cm−1 (\\OH) and 1695–1654 cm−1 (C_O) compared
with diesel. They claimed that the polar oxygen functional groups in
the CC would bond with the oxygen groups on oxidized coal surfaces
through hydrogen bonding as well as the residual non-polar hydropho-
bic groups in the CC would bond with the non-polar groups on oxidized
coal surfaces by hydrophobic function. Consequently, they claimed
that the floatability of the oxidized coal was greatly improved by the
coverage of the CC on the oxidized coal surface while the polar groups
on the oxidized coal surfaces were fully passivated. However, further
studies into which is the first action for the polar oxygen functional
groups and non-polar hydrophobic groups to bond with the oxidized
coal surface may be paid more attention. The selectively of the CC
could be combined with the mechanism of the adsorption of the CC
on the oxidized coal surface.
8 B. Wen et al. / Powder Technology 319 (2017) 1–11

Fig. 10. FTIR spectrum of oxygenated polar compound collector (CC) and diesel [89].

Gui et al. [90] also paid an attention into the effective flotation of
oxidized coal using an oxygen-containing collector α-furylacrylic
acid. They compared the flotation recovery of oxidized coal using
α-furylacrylic acid and dodecane as the collector, respectively. The
flotation performance was much better using α-furylacrylic acid as
the collector than using the dodecane. They used the zeta potential,
FTIR and surface free energy analysis to indicate the mechanism
of the effective adsorption of α-furylacrylic acid on the oxidized
coal surface, as shown in Fig. 11. They claimed that the dodecane
could only adsorb at the hydrophobic sites on the coal surface. For
α-furylacrylic acid, it could bond with the oxidized coal surface through
hydration film. In other words, a repulsive hydration force existed
between oxidized coal and α-furylacrylic acid. α-Furanacrylic acid
could not directly form hydrogen bonds with the oxygen-containing
functional groups on the coal surface but the water molecules in
hydration film acted as the bridging role of hydrogen bond for the ab-
sorption of α-furanacrylic acid on oxidized coal surface. For the gangue
particles in coal flotation, the surface of gangue may be also covered
by the hydration film and the gangue surface may be also adsorbed
by α-furanacrylic acid. The interaction between gangue surface and
α-furanacrylic acid may be paid further attention to qualify the selec-
tivity of α-furanacrylic acid in oxidized coal flotation.
In the 21st century, biotechnology has been developed and ap-
plied in many industrial fields. The bio-separation processes of min-
erals have also been developed, such as bio-desulfurization of high
sulfur coal, bio-flocculation and bio-flotation [91–96]. In the process
of bio-flotation, the conventional flotation reagents, such as Methyl
Isobutyl Carbinol, diesel may be replaced by bacteria. However, the
bio-flotation of coal attracts less attention.
Recently, Ramos-Escobedo et al. [79] investigated the flotation of
coal using the bacteria of Staphylococcus carnosus as bio-collector
which was proved to effectively enhance the surface hydrophobicity
of bituminous coal from Rio Escondido Basin. They used SEM and FTIR
to indicate the interaction between the bacteria of Staphylococcus
carnosus and the coal surface. As shown in Fig. 12, the adhesion of
bacteria on the coal surface started individually in the first 2 h, then
the bacteria were observed in monolayers after 6 h. At last, the bacteria
began to agglomerate in multiple layers. Through the FTIR analysis,
the\\CH2 functional group was found on the surface of bacteria. It indi-
cated that the bacteria could selectively adhere to the hydrophobic sites
on the coal surface and built a biofilm formation on the surface of
the coal. The biofilm was formed by fatty acids and polysaccharides,
which made a difference in the surface properties between coal and
minerals. However, the disadvantage of bio-flotation was the long
working time and high economic cost, which should be paid more
efforts to solve.
As is known, low rank/oxidized coal surface has amounts of oxygen-
containing functional groups which are the main negative factors re-
ducing the surface hydrophobicity of coal surface. If the special bacteria
can be bonded with these oxygen-containing functional groups on low
rank coal surface, the improvements in the hydrophobicity of low rank/
oxidized coal surface can be achieved. In addition, the special bacteria

Fig. 11. The interaction schematic diagram between dodecane/α-furylacrylic acid and oxidized coal surface [90].
 B. Wen et al. / Powder Technology 319 (2017) 1–11
Fig. 12. SEM photomicrographs of bacteria of Staphylococcus carnosus adhering to coal surface at different times in a medium of pH = 9. Time adhesion: (a) 0 h, (b) 1 h, (c) 2 h, (d) 6 h,
(e) 12 h and (f) 24 h [79].
should have its selectivity of adsorption such as the bacteria have its
hobby especially on the oxygen-containing functional groups (\\C\\O,
\\C_O, COOH) on the coal surface. According to this strategy, the
surface hydrophobicity of low rank/oxidized coals can be eventually
improved. Further studies into these special bacteria for effectively
collecting low rank/oxidized coals are needed.
5. Summary
(1) The flotation of low rank/oxidized coals is a key issue in the coal
preparation industry and energy supply. However, the surface
hydrophobicity of low rank/oxidized coal is relatively low and
hence they are difficult to float using both the common oily
collectors and conventional flotation technologies. As the de-
mand for energy supply increases, low rank/oxidized coals
should be utilized.
(2) The emulsion of oily collectors by surfactants not only enhances
the surface hydrophobicity of low rank/oxidized coals but also
reduces the collector dosage required in coal flotation. The
floatability of low rank/oxidized coals can be improved by both
9
emulsified oily collectors and the addition of surfactants. The
mixture of surfactants and oily collectors are economic and effec-
tive for the flotation of low rank/oxidized coals.
(3) Because low rank/oxidized coals have amounts of oxygen-
containing functional groups, introducing both the oxygen-
containing functional groups and aromatic hydrocarbons into
the oily collectors becomes a good way to produce some effective
collectors, such as oxidized diesel, α-furylacrylic acid and THF
esters. These effective collectors can bond with low rank/
oxidized coal surface through hydrogen bonding, π-bonding,
and hydrophobic bonding.
(4) Converting vegetable oil/waste oil into biodiesel or other oily
products as coal flotation collector is environmentally friendly
and sustainable. The biodiesel contains both hydrocarbon
oils and fatty oils. In addition, there are amounts of oxygen-
containing functional groups in biodiesel which can be easier
bonded with the oxygen-containing functional groups on coal
surface. In addition, the creation of bio-collector, such as bacteria
may be a new way to solve low rank/oxidized coals flotation in
the future.
10 B. Wen et al. / Powder Technology 319 (2017) 1–11
Acknowledgements
This work was supported by the Fundamental Research Funds for
the Central Universities (2017BSCXA06).
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