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Accepted Manuscript

Title: Highly efficient and recyclable depth filtrating system


using structured kapok filters for oil removal and recovery
from wastewater

Author: Ting Dong Shengbin Cao Guangbiao Xu

PII: S0304-3894(16)30902-5
DOI: http://dx.doi.org/doi:10.1016/j.jhazmat.2016.10.005
Reference: HAZMAT 18086

To appear in: Journal of Hazardous Materials

Received date: 27-6-2016


Revised date: 9-9-2016
Accepted date: 2-10-2016

Please cite this article as: Ting Dong, Shengbin Cao, Guangbiao Xu, Highly
efficient and recyclable depth filtrating system using structured kapok filters
for oil removal and recovery from wastewater, Journal of Hazardous Materials
http://dx.doi.org/10.1016/j.jhazmat.2016.10.005

This is a PDF file of an unedited manuscript that has been accepted for publication.
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Title:

Highly efficient and recyclable depth filtrating system using structured kapok filters for oil removal

and recovery from wastewater

Authors and affiliations:

Ting Dong 1, Shengbin Cao1,2, Guangbiao Xu 1,3*

1. College of Textiles, Donghua University, Shanghai 201620, China

2. School of Mechanical Engineering, Shanghai Dianji University, Shanghai 201306, China

3. Key Laboratory of Textile Science and Technology Ministry of Education, Donghua University,

Shanghai 201620, China

4.

*Corresponding author contact information: (86) 021-67792631, guangbiao_xu@dhu.edu.cn

Present/permanent address:

Room 3023, Building 3, College of Textiles, Donghua University, 2999 North Renmin Road,

Songjiang district, Shanghai 201620, China

1
Graphical abstract

Highlights

 A depth filtrating system is designed to remove and recover oil from wastewater.

 The filter media is 3D kapok fibers prepared by the air-laying-bonding method.

 Oil removed from wastewater is subsequently recovered by centrifugation.

 High oil/water separation, water and oil reclamation, and excellent cyclic usability.

 The filter’s structure and properties of model oils play important role in the process.

Abstract

A depth filtrating system with rotatable and taper-shaped filter column was reported to highly

remove and recover oil from wastewater. In the work, structure filters made of kapok fibers were

prepared by air-laying-bonding method. The oil removed from wastewater was then recovered from

the oil-loaded filter by rotating the filter column, and the resulted filter was reused. The filtrating

system demonstrated extremely high oil/water separation in which oil was completely retained by the

filter at the first 20-100 min while water passed through the filter’s body with a flow rate of 560

mL/min using 11500 - 13150 mg/L vegetable oil or diesel polluted water. A total of 47.6-176.4 L
2
clean water was collected after four cycles of filtration and centrifugation. The separating process

depended on filter’s structure (packing density) and properties of model oils. The wetted filters

which absorbed up to 795.6 g (32.31 g/g) of oils were centrifuged to recover 80-91 % of the oils. The

sorption capacity appeared to become constant until 4 cycles of filtration after an apparent drop of

1-6 g/g in the second cycle, because of unrecoverable residual oil (2-5 g/g). The decrease of flow

rates was favorable to filtration of low viscous oil.

Keywords: Oily wastewater; Depth filtration; Kapok fiber; Recovery system; Reusability

1. Introduction

Oily wastewater is one of the environmental concerns today. As one of the most important global

sources of energy and raw material for industries, any oil spillage or inefficient extraction implies not

only environmental issues but also economic loss [1]. By now, various technologies, such as

absorption, filtration, membrane technology and physical, mechanical, biological and photochemical

method were proposed for oily wastewater treatment [2, 3]. The most commonly way is done by

absorption or filtration using porous sorbents [4]. A large number of synthetic polymers including

polypropylene, polyester, polyurethane and various acrylic and olefin resin have been reported as the

oil sorbents with high capacity of oil absorption [5-7]. However, these synthetic products are

generally made from oil byproducts and are non-renewable and nondegradable. Natural sorbents are

thus gaining interests as the alternatives. These materials are derived either from animal and plant

residues (organic sorbent) or minerals (inorganic sorbent). Natural inorganic materials are less

preferred due to their low buoyancies and oil sorption capacities [8]. Organic fibrous materials, like

3
cotton [9], milkwood [10], silk-floss fiber [11], cattail [12] and populus seed fiber [13], show great

advantage, such as relatively high oil absorption, biodegradability, richness in nature and

cost-effectiveness.

Kapok fiber is a natural cellulosic fiber with a waxy surface [14]. Single kapok fiber showed a huge

hollow lumen which differentiates the fiber from others and endows it with porosity high up to 90 %.

Kapok fiber and kapok-based materials were reported to be used in various fields. Typically, kapok

fiber was used as stuffing in bedding, upholstery, life preservers and other water-safety equipment

because of its excellent buoyancy [15]. It was also suggested as excellent insulation material against

heat and sound because of its air-filled lumen [16]. As an important type of cellulosic plant fiber,

kapok fiber has been employed as a reinforcing material in polyester matrixes [17]. Due to its natural

microtube structure, kapok fiber was used as the natural template to fabricate hollow metal-oxide

fibers [18, 19]. It was also considered as a potential starting material for the preparation of versatile

activated carbon fibers [20], and as a biocompatible drug and catalyst carrier [21].

Owing to its hollow lumen and waxy surface, kapok fiber was appreciated as the natural sorbent for

oil spill cleanup [10, 22-25] including inland oil spill remediation [26]. It was also reported to be

chemically modified or coated to show a new lipophilic property with varied oil sorption capacity

[22, 27, 28]. Being one of the researches, we have had researched on kapok fiber since 2003. As for

oil sorption purpose, the hollow structure of kapok fiber is beneficial due to its large effective pore

volume, and the waxy surface can enhance its adherence to oils. We characterized different oil

adsorption and adhesion of kapok fiber by size and adhesive energy distribution of oil droplets

adsorbed on single fiber [29], finding that kapok fiber adsorbed different oils with average droplet

size varying from emulsified state (0.1-25 μm) to dispersed state (25-100 μm). The average adhesive

energies between kapok fiber and oils were around three times stronger than that between polyester

fiber and oils. During oil sorption process, the oils are firstly adsorbed onto kapok fiber by

hydrophobic interactions and van der Waals forces between oils and the waxy surface, and then enter

4
the kapok assemblies and penetrate into the kapok lumens through internal capillary movement [30].

The amount of oil absorbed and retained by kapok assemblies depend on the available pores

contributed by inter-fiber distances and fiber’s lumens, and the physical characteristics of the model

oils including but not limited to viscosity density, surface tension and its contact angle with kapok

surfaces. With increasing the packing density, the oil sorption capacity of kapok assemblies

decreased as the total void fraction inside the kapok microstructure is decreased. Furthermore, a

dual-scale model based on Washburn Capillary Theory was developed to study the oil sorption

behavior of kapok assemblies with relation of the pore structure [31]. With increasing the packing

density, the ratio of pores contributed by lumens of kapok was increased. At the tightly packed

condition of 0.10 g/cm3, oil absorbed by kapok lumens accounted for up to one fifth of the total oil

absorption of kapok assembly. Study showed that chloroform treatment was detrimental to the fibers’

oil absorption by 2.1% of reduction for the damaged waxy coating [22], but our work revealed that

an appropriate chloroform treatment could markedly increase the oil sorption rate due to its highly

roughened surfaces [30].

Although various materials as well as technologies were proposed to remove the spilled or residual

oil from wastewater, hardly any paid attention to the recovery of oil during the removal. In the work,

a depth filtrating system characterized with rotatable and taper-shaped filter column was reported to

highly remove as well as recover oil from wastewater. Since oil removal efficiency depends on the

quality of filter bed media, three-dimensional structured kapok filters with controllable porous

structure was prepared based our previous work by air-laying-bonding method [32]. During the work,

the oil removed from wastewater was then recovered from the oil-loaded filter by rotating the filter

column, and the resulted kapok filter was reused in the subsequent filtration. The mechanism of

separating process was investigated. The results demonstrated the extremely high efficiency of the

system in oil removal and recovery, showing great economic and environmental significance and

advantage to other technologies.

5
2. Materials and methods

2.1 Materials

Kapok fibers used in the work are java kapok growing up in Pate County, Java Tengah, Indonesia.

Characterization of kapok fibers has been previously described and is summarized in Table 1. The

fiber has a hollow structure with wall thickness of 1±0.16μm. The external diameter of the fiber

varies from 9.82 μm to 22.28 μm with an average value at 16.29±2.7μm [31]. Copious of waxes on

the fiber’s surface makes it excellent hydrophobic. The surface energy of kapok fiber is only 40.64

mN/m with most of that contributed by dispersion components. During preparation of kapok fiber

filters, a kind of polypropylene/polyethylene sheath-core composite fiber (ES) which has a

low-melting-point sheath of about 130 ℃ and strong and heat-resistant core was employed to bond

kapok fibers. Vegetable oil and diesel were chosen as experimental oils. Properties of the oils are

listed in Table 2.

2.2 Fabrication of structured fiber filters

The preparation of kapok filters was based our previous work by air-laying-bonding method [32].

Kapok fibers were firstly blended with 20 % ES, and carded into fibrous web through an air-forming

machine (40B, Rando, USA). As prepared fibrous web was then filled layer by layer in a perforated

steel mould. The mould is produced according to the shape of filter column where kapok filter is

hold during filtration. The fibers in the mould were thermally bonded by application of hot-air at

140 ℃ in the electro-thermostatic drying oven (DGG-9030A, SUMSUNG, China). After 60 - 90 min

heating, structured kapok filters were formed. The porous structure of the filters was controlled by
6
packing densities with different amount of fibers filled in the mould. Three packing densities (0.010

g/cm3, 0.015 g/cm3 and 0.020 g/cm3) were investigated.

2.3 Experimental setup and filtration procedures

The filtration equipment is showed in Fig.1. Oil and tap water were separately poured into tank (1)

and tank (2). The pump (11) and (12) carried the liquids toward the sieve (3), where stable liquid

capacities were controlled. The water blended with oil was sprayed at a constant load through the

sieve to filter column (5). The filter column is rotatable and tapered shaped with an incline of 17.2°.

The height and diameter of the upper and the lower face are 10.5 cm, 17.8 cm and 11.5cm,

respectively. The runoff was filtrated by kapok filter (6) with varied packing density. Afterwards, the

water was collected in container (10) and disk-like kapok fiber pads which were produced according

to the method described in section 2.2 were used to absorb floated oil on the collected water by every

5 min. The pads were then placed in room environment for 24 h allowing the evaporation of

adsorbed water on the pads’ surfaces. A contrast experiment in which a pad adsorbing trace of pure

water was sustained in the same condition was carried out to confirm the complete evaporation of

water. The oil concentrations in the water samples were calculated based on the mass change of the

pads. During the process, the time when a visible blob of free-phase oil was appeared in the collected

water was defined as the breakage of oil through the kapok filter [23, 24].

The filtration was stopped when apparent oil leakage was happened. The filter column with

oil-loaded kapok filter was subsequently covered with steel tap and subjected to the rotation of 1440

r/min driven by the electromotor (13). The absorbed oil with some amount of water was thus

centrifuged from the kapok filter and entered into container (9) via the (15) and the buffer space (7)

between the outer column (4) and the filter column (5). The centrifugal times of vegetable oil- and

diesel-loaded filters were separately 7 min and 30 s. The resulted kapok filter was then reused in the

7
next filtration. To avoid possible air trapping within the kapok filter as well as to wash off oils coated

on apparatus walls, the kapok filters were previous filtrated with pure water for 5 min using

increased water flow rates, before starting a new cycle of oily water separation.

2.4 Measurements

The filtration efficiency was evaluated in every five-minute by equation (1).

moin  moout
Filtrating efficiency = 100% (1)
moin
Where moin is the oil mass in runoff before the filter. moout is the oil mass measured in collected water.

The mass of oil and water absorbed by kapok filters during filtration were calculated by equations

(2-3).

mo
Oil sorption capacity = (2)
mf
mw
Water sorption capacity= (3)
mf

mo  m fow  m f  mw
(4)

m f is the mass of dry filters before filtration. m fow is the mass of wetted filters after filtration. mo

and mw are masses of absorbed oil and water, respectively. The values of m f and m fow are

directly weighed. During the centrifugation process, water was observed to be thrown out quickly

from the wetted filters in the first few seconds, while oil was drained out gradually from the filters

with decreased rate. Therefore, mw is measured according to the volume of water collected after

centrifugation of the wetted filters and mo is then calculated by equation (4).

The efficiencies of liquid removal and oil recovery from the wetted filters in the centrifugation

process were evaluated by equations (5-6).

8
m fow  m fowi
Liquid removal = 100% (5)
m fow

m fowi  mw  m f
Oil recovery = 100% (6)
mo
m fowi  m f
Residual oil = (7)
mo

m fowi is the mass of filters after being subjected to i seconds or minutes of centrifugation. Liquid

removal presents the percentage between the mass of liquids removed by centrifugation and the total

mass of the wetted filters. Oil recovery presents the percentage between the mass of oil recovered by

centrifugation and the total mass of oil absorbed by the filters. The mass of residue oil after being

subjected different times of centrifugation was also evaluated using equation (7).

3. Results and discussion

3.1 structured kapok filters

The hollow structure of kapok fiber endow it a porosity of 77 %. The fibers are pretty fluffy with

0.305 g/cm3 in bulk density considering its large lumens [31]. Therefore, instead of mechanical force,

air-flow was employed to manipulate the fibers in web forming and bonding in order to minimize

damage of fibers. Fig.2 presents a photo of shaped kapok filter and its typical SEM images which

were characterized by SEM (TM3000, Hitachi, Japan). As can be observed in the SEM images, the

low heat-tolerant sheath of ES was fused under the temperature of 140 ℃, leaving a strong core to

connect and bond kapok fibers surrounding it to form a structured porous filter.

3.2 Preliminary filtration

9
Oil concentration in the runoff was 11500 - 13150 mg/L. The experiment began with filtration of

viscous vegetable oil by kapok filter of 0.02 g/cm3, because this is considered as a situation in which

the closely packed filters is more likely to become clogged by the increased pressure losses. As

shown in Fig.3, kapok filter was clogged within 30 min (the water just accumulated over the kapok

filter) when water in-flow rate was higher than 700 mL/min. The gradually accumulated oil in the

filter’s pores also led to the clog despite of unhindered filtration before the first 55 min with water

in-flow rate at 600 mL/min. As the water in-flow rate was decreased to 560 mL/min, a stable and

continuous filtration process was obtained. The experiment was finally stopped because the oil broke

through the filter’s body appearing in the collected water. Therefore, a water in-flow rate of 560

mL/min was chosen and maintain for the later experiments.

3.3 Cyclic filtration and recovery

3.3.1 Filtration performance

Table 3 and Table 4 summarize the results of kapok filters in four times of centrifugation and cyclic

filtration with vegetable oil and diesel as the experimental oils, respectively. In the first cycle,

filtration of vegetable oil and diesel separately lasted for 100 min and 60 min after which the oils

broke through the filter’s body (0.02 g/cm3) starting to appear in collected water. After oil

breakthrough, a sharply aggravated oil leakage occurred with the filtrating efficiencies decreased to

only 45-80 % in other two five-minute durations, as shown in Fig.4. A total of 53.2 L and 30.8 L of

clean water were collected for vegetable oil and diesel, respectively. With decreasing packing

density, the time of oil breakthrough was decreased by 10-40 min. At 0.01 g/cm3, there were 30.8 L

and 14.0 L of clean water collected for vegetable oil and diesel, respectively.

The lagging movement between oil and water through the filter’s body is a result of different
10
physical interactions between the fibers and two liquids [23, 24]. As demonstrated by contact angles

in table 1 and 2, kapok fiber is highly oleophlic and hydrophobic. When oil/water runoff entered the

filter column, water was repelled by hydrophobic kapok fiber and pass through pore spaces between

fibers under gravity. It was observed that some water just rolled off from the filter’s surface and gone

through space between the filter and the wall of filter column. In contrast, oil drops coming into

contact with the kapok fibers were absorbed and coated on the fibers immediately. The breakthrough

of oil was significantly influenced by the available sorption surfaces and sorption capacity of the

kapok filters and also the property of the oil. Apparently, the filters with a higher packing density

could provide more sorption surfaces and larger oil pickup, thus showing longer duration of filtration

before oil breakthrough. Comparing with diesel and vegetable oil, the differences in oil’s property

and their interactions with kapok fibers were believed to be reasons causing difference in oil

breakthrough. When a liquid interacts with a solid surface, wetting and adhesion processes determine

its separating behavior [33]. Apparently, the bad wettability and adhesiveness between oil and fiber

can lead to easy escape of oil droplets from pores of fibrous filter to outflow, as illustrated in Fig.5 a.

For case in Fig.5 b, oil droplets are attached on fiber of good oil wettability, but easily deform and

detach again due to the bad adhesiveness of fiber with it. However in Fig.5 c, a large number of oil

droplets are captured and retained by the fiber which has both excellent adsorption and adhesion to

the oil. The interactions of diesel and vegetable oil with kapok fibers were just falling into cases in

Fig.5 b and c, respectively. The contact angles of kapok with diesel and vegetable oil were less than

60° (in table 2), but the average droplet adhesive energies of vegetable oil and diesel with kapok

fibers were 9.40×10-11 J and 3.78×10-11 J, respectively [29]. The bad adhesion of diesel with kapok

fiber combined with its low viscous property could cause it ready to deformation, detachment and

transfer within the kapok filter body, and thus quicker to break through filter body occurring in the

collected water.

During the following cyclic filtrations, a decrease of 5-25 min in oil breakthrough was observed for

11
both oils. There was 39.2 L and 25.2 L of clean water collected separately for filtration of vegetable

oil and diesel in the fourth cycle when oil broke through at 75 min and 50 min, respectively. The

unrecoverable residual oil trapped in the filter’s body (shown in table 3 and table 4) which reduced

subsequent capacity for oil pickup was believed to be one of the main factors causing premature oil

breakthrough of the reused filters. In addition, irreversible deformation of kapok filter after the oil

drained out by the centrifugal force was another important reason for that.

3.3.2 Comparison of absorbed oil and water in the wetted kapok filters

The absorbed oil and water by the wetted kapok filters in different filtration cycles are compared in

Fig.6. Sorption efficiency of a sorbent by experiments using oil separator or in dynamic mode was

deteriorated and generally far lower than that measured under static sorption conditions [34].

However, we find that 25.50-32.31 g/g of vegetable oil and 14.42-17.37 g/g of diesel were absorbed

by kapok filters with different packing density from runoff during the first cycle of filtration. There

was a decrease of 1-6 g/g in oil sorption capacity in the second cycle, after which the sorption

capacity appeared to become constant until 4 cycles of filtration. Actually, we found that the filters

with higher packing density (0.02 g/cm3) could be reused for 10 or more times without apparent

reduction in sorption efficiency. However, the structure of filter with low packing density (0.01

g/cm3) would be easier to be damaged under the centrifugation. As a result, numbers of reuse was

reduced. Reusability of kapok fiber has been investigated by centrifugation at 3000 rpm [25] and by

vacuum pump at 525 mbar [22]. In the cycles of sorption/desorption, significant decreases in oil

sorption capacity were also reported to occur in the second cycle. From the second cycle to the fourth

[25] or even to the fifteenth cycle [22], no significant changes in the sorption capacity were observed.

The significant reduction in the second cycle has been proposed [22, 25]. This sudden drop from the

first and the second cycle was due to irreversible deformation as 2-5 g of oils still trapped in per

12
gram fibers (in table 3 and 4) after centrifugation. The continuous deformation due to this remaining

oil in the kapok filters, affected the capacity of kapok to absorb more oil in the subsequent cycle. In

addition, there was no apparent change showed in the bulk volume of the filter after four cycles of

centrifugation, but some local deformations, inside the filter were irreversibly formed once oil

drained out. The main deformation of filter was observed to be the transfer of central fiber to

outwards. This change of inner porous structure then caused reduction of subsequent oil sorption.

Compared with other data from runoff experiments, the sorption capacities of wool waste filler and

reed filler were separately 0.85 g/g and 0.30 g/g despite of high efficient achieved (98-99 %) in oil

removal from runoff under a 10 m/h filtering rate [34]. Kapok fiber, cattail fiber, polyester fiber,

wood ship and rice husk were reported to absorb more than 70 % of oils from gas station runoff

under high water flow rate of 20 L/min. However, sorption capacities of these sorbents were 0.83 g/g,

1.11 g/g, 1.10 g/g, 0.34 g/g and 0.30 g/g respectively [11]. Instead of densely packed filter fillers, the

extremely high porosity of kapok filter (98.5-99.2 %) is one important reason distinguishing our high

efficiency form the data discussed above. In addition, the more uniformly porous microstructure of

kapok filter contributed by the application of air-laying-bonding can form well-proportioned internal

capillary force which allows oil to penetrate and migrate through pores. As a result, high oil retention

and sorption efficiencies could be achieved. For densely packed fillers, less space is available for oil

storage. More importantly, the structure and stability of pores inside the filters differ significantly.

As a result, some large pores within loose kapok fibers do not have sufficient capillary force to retain

oils, as the capillary pressure in a pore is inversely related with the pore’s size.

In contrast to oils, the water absorbed by kapok filters was just among 1.63-8.53 g per gram fibers.

The distinctive selectivity of kapok filters in oil-to-water was associated with the chemical

characteristics of kapok fibers. It was reported that there were waxes by about 3 % coating on

kapok’s surfaces [22]. The low surface energy and non-polar actions (in table 1) make kapok fibers

highly oleophlic and hydrophobic where affinities between oil molecules and fiber surface are much

13
higher than that between water molecules and fiber surface. Moreover, the volume of absorbed water

was inversely changed with variation in absorbed oil, which implied gradually displacement of oil to

water and its occupation in the kapok filter body.

3.3.3 Centrifugation and recovery

Fig.7 shows the liquid removal and oil recovery of kapok filters as a function of centrifuging time

during the first cycle of centrifugation. The vegetable oil- and diesel-loaded filters took separately 7

min and 30 s to reach the balance points where masses of the wetted filters were hardly changed after

being subjected to a longer duration of centrifugation. The easily drain out of diesel is because the

viscosity of diesel is quiet low. Another important reason, as shown in our previous study, is that the

adhesive energy between diesel and kapok fiber is also significantly low, which is near one third of

that between vegetable oil and kapok fiber [29].

There were 81-89 % of liquids removed from the filters in balance positions and accordingly 75-91 %

of oils recovered (in table 3 and 4). Fig 8 and 9 showed the micro-distribution of diesel and vegetable

oil in the voids of kapok filters after different duration of centrifugation. The oil uptake between

kapok fibrous network and within the fibers’ lumen via sorption are dominant mechanisms causing

oil retention and separation from runoff. When subjected to rotating centrifugation, a majority of oil

retained between the network was ready to be drained out (images a and b), while oil uptake within

the lumens was difficult to be drained out even subjected to long duration of centrifugation (images c

and d). This explained why there were still around 2-5 g of residual oil in per gram fibers (in table 3

and 4). The recovered vegetable oil and diesel with some amount of water deposited in the bottom

for the first cycle of filtration is shown in Fig.10. At the highest packing density of 0.02 g/cm3, 421.2

g of diesel and 722.4 g of vegetable oil were recovered. The increase of packing density was found to

exerted little influence on the centrifugation of the two oils. This was because the constriction of

14
channel flow sizes at higher packing density was not favorable for the drain out of oils, but the more

oil it loaded resulted in stronger centrifugal force. Generally, the total amount of oils collected after

filtration was 2.9-9.1 g lower than oils loaded in runoff before filtration. This was attributed to oils

coated on apparatus walls.

3.4 Influence of filtrating rate

The filtration results of low viscous diesel by kapok filters, in particular under low packing condition

were not so desirable. Another experiment for diesel polluted water was therefore performed under

different water-flow rates with kapok’s packing density at 0.010 g/cm3. The flow velocity directly

affects the amount of shear force on oil drops and therefore their deformation and transfer within the

filter body [35]. The result showed that the decrease in water flow rates would improve the filter’s

filtration to low viscous oil (in Fig.11). At 560 mL/min of water flow rate, the diesel took 30 min to

break through the kapok filter when 14 L of clean water was collected. The breakthrough was

postponed to 50 and 75 min when water flowed separately at 450 and 360 mL/min, and as a result

20.25 and 25.20 L of clean water were collected, respectively. Also, there are 5-8 g/g increases in oil

sorption capacity of the filters, but no obvious changes in others namely water absorption, liquids

removal and oil recovery.

4. Conclusions

Highly efficient and recyclable depth filtrating system using structured kapok filters was

demonstrated to be an effective way to recycle oil from oily wastewater. The high efficiency of the

work is respected on two aspects: high efficiency to absorb oil from wastewater and high efficiency

15
to recover oil from the filter. Instead of densely packed filter fillers suggested by literatures, the

extremely high porosity (98.5-99.2 %) and the more uniform microstructure of kapok filter

contributed by the application of air-laying-bonding were major mechanism contributing to high

efficiency.

In the work, oil was completely retained at the first 20-100 min while water passed through the

filter’s body with a flow flux of 560 mL/min using 11500 - 13150 mg/L oil polluted water. A total of

47.6-176.4 L clean water was collected after four cycles of filtration and centrifugation. The

separating process was affected by filter’s structure (packing density). Filters with a higher packing

density could provide more sorption surfaces and larger oil pickup. As a result, the time of oil

breakthrough was decreased by 10-40 min with packing density decreasing from 0.02 g/cm3 to 0.01

g/cm3. The wetted filters can efficiently absorbed up to 795.6 g (32.31 g/g) of oils during the first

cycle of filtration. The oil sorption capacity appeared to become constant until 4 cycles of filtration

after an apparent drop of 1-6 g/g in the second cycle, because of unrecoverable residual oil of 2-5 g/g.

75-91 % of oils were recovered by 30 s (diesel) or 7 min (vegetable oil) of centrifugation at 1440

r/min. For example, 421.2 g of diesel and 722.4 g of vegetable oil were recovered by kapok filter

(0.02 g/cm3) in one cycle with separately 59 g and 80.5 g of water deposited in the bottom of

container.

Compared with the conventional, established technologies such as diffused air flotation,

electro-flotation, etc, which may remove oil from oil/water emulsion in continuous mode, the

purpose of this work is to utilize natural fibers as effective filtering material recycling oil from heavy

oil contaminated waters, such as the thin film of spilled oil which may has been treated with sorbents

or other technologies. This does not require high operating cost and complex operation, such as

coagulants/flocculants involved.

Acknowledgment
16
The research is financially supported by “the Fundamental Research Funds for the Central

Universities” (numbered by 15D110105), and “Donghua university doctorial innovation fund for

2014~2015” (numbered by CUSF-DH-D-2015003).

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19
Figure captions

Fig.1 Filtration setup: (1) oil vessel; (2) water tank; (3) sprinkler head; (4) cylindrical outer column;

(5) rotatable inner column with tapered shape; (6) fiber filter; (7) buffer for recovered oil; (8)

perforated baseboard supporting the filter; (9) recovered oil; (10) collected water; (11) pump

controlling oil; (12) pump controlling water; (13) electromotor driving the rotation of tapered inner

column; (14) driving gears (15) oil discharge outlet.

Fig.2 (a) three-dimensional morphology and (b) SEM images of kapok filters with packing density at

0.02 g/cm3

Fig.3 Filtration of vegetable oil polluted water under different water flow rates, PD=kapok’s packing

density.

Fig.4 Oil removal efficiency as a function of filtrating time: (a) vegetable oil, (b) diesel, PD=

kapok’s packing density.

Fig.5 Separating process of oil from water (a) oil droplets escaped from pores of fiber filter to

outflow for the bad wetting and adhesiveness between oil and fiber, (b) oil droplets attached on fiber

surface of good wettability but deformed and detached again due to its bad adhesiveness with the

fiber, (c) oil droplets adhesion and coalescence on fiber which has both excellent adsorption and

adhesiveness with the oil.

Fig.6 Comparison of absorbed oil and water by the wetted kapok filters in each filtration cycle,

PD=kapok’s packing density.

Fig.7 Liquid removal and oil recovery as a function of centrifuging time during the first cycle: (a)

vegetable oil, (b) diesel, PD=kapok’s packing density.

Fig.8 Distribution of vegetable oil in the voids of kapok filters after different duration of

centrifugation: (a) 1min, (b) 3min, (c) 5min, (d) 7min.

Fig.9 Distribution of diesel in the voids of kapok filters after different duration of centrifugation: (a)

20
0s, (b) 10s, (c) 20s, (d) 30s.

Fig.10 Recovered vegetable oil (upside) and diesel (downside) with some amount of water deposited

in the bottom during the first cycle of filtration, (a1) and (a2) kapok’s packing density=0.020g/cm3,

(b1) and (b2) kapok’s packing density=0.015g/cm3, (c1) and (c2) kapok’s packing

density=0.010g/cm3.

Fig.11 Filtration of diesel polluted water under different water flow rates, PD=kapok’s packing

density.

21
Fig.1

22
Fig.2

23
Fig.3

24
Fig.4

25
Fig.5

26
Fig.6

27
Fig.7

28
Fig.8

29
Fig.9

30
Fig.10

31
Fig.11

32
Table 1Characteristics of kapok fiber a
Surface energy (mN/m)
External diameter wall thickness Pulling staple Water contact
Dispersion Polar
(um) (um) length (mm) angle (°)
components components
16.29±2.72 1.00±0.16 22.00±1.28 146.38±2.63 33.04 7.60
a
data coming from previous study [30, 31].

33
Table 2 Properties of experimental oils
Density Viscosity Surface tension Contact angle with
Oil type
(g/cm3) (mPa·s) (mN/m) kapok fiber (°) a
Diesel 0.85 10.00 28.22 36.98
Vegetable oil 0.92 72.10 33.45 50.97
a
data coming from previous study [29].

34
Table 3 Cyclic filtration of runoff with vegetable oil as the experimental oil
Collected
Packing Number Oil Liquid Oil Residual
clean
density of breakthrough removal recovery oil
3 water
(g/cm ) cycles (min) (%) (%) (g/g)
(L)
1 60 30.8 87.85 88.61 3.68
2 50 25.2 85.21 85.37 4.42
0.010
3 50 25.2 85.21 85.99 4.58
4 40 19.6 83.94 83.34 4.41

1 90 47.6 88.38 90.15 3.03


2 70 36.4 84.50 86.04 3.41
0.015
3 70 36.4 83.56 84.88 3.70
4 70 36.4 84.83 86.35 3.31

1 100 53.2 86.99 89.47 2.69


2 80 42.0 83.61 86.33 2.83
0.020
3 80 42.0 83.28 86.02 2.86
4 75 39.2 83.39 85.98 2.69

35
Table 4 Cyclic filtration of runoff with diesel as the experimental oil
Collected
Packing Number Oil Liquid Oil Residual
clean
density of breakthrough removal recovery oil
3 water
(g/cm ) cycles (min) (%) (%) (g/g)
(L)
1 30 14 83.24 80.30 3.42
2 30 14 83.28 80.23 3.35
0.010
3 20 8.4 81.95 75.24 2.82
4 25 11.2 83.79 80.19 2.82

1 40 19.6 82.20 81.83 2.62


2 40 19.6 82.76 82.68 2.48
0.015
3 35 16.8 81.09 79.76 2.65
4 30 14 81.88 81.66 2.09

1 60 30.8 82.12 84.46 2.48


2 50 25.2 81.64 83.89 2.18
0.020
3 50 25.2 81.50 83.45 2.19
4 50 25.2 81.18 83.14 2.26

36

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