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A Protein-Functionalized Microfiber/Protein Nanofiber Bi-layered Air Filter

with Synergistically Enhanced Filtration Performance by a Viable Method

Article  in  Separation and Purification Technology · July 2019

DOI: 10.1016/j.seppur.2019.115837

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 Separation and Purification Technology 229 (2019) 115837

Contents lists available at ScienceDirect

Separation and Purification Technology

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

A protein-functionalized microfiber/protein nanofiber Bi-layered air filter T

with synergistically enhanced filtration performance by a viable method
⁎ ⁎
Juejing Liua, Francis O. Dunnea, Xin Fanb, Xuewei Fua, , Wei-Hong Zhonga,
a
School of Mechanical and Materials Engineering, Washington State University, Pullman, WA 99164, USA
b
College of Food Science and Technology, Huazhong Agricultural University, Wuhan, Hubei 430070, China

A R T I C LE I N FO A B S T R A C T

Keywords: Realization of high filtration efficiency and low pressure drop is in critical need for advanced air filters.
Protein-functionalization Electrospun nanofiber-based air filters create high surface area which can efficiently capture pollutants, but the
Cotton fiber production rate is difficult to improve and it’s challenging to reduce the pressure drop. In this study, we de-
Protein nanofiber monstrate that a protein-functionalized cotton-fiber composite air filter with high filtration efficiency and low
Evaporation-controlled assembly
normalized pressure drop can be fabricated via an evaporation-controlled strategy. It is the first report that a
Bi-layered air filter
“green” solvent system (ethanol aqueous), an optimized protein concentration, and evaporation temperature can
lead to protein-functionalized cotton filters with improved air filtration efficiency. The resulting loose micro-
fibrous structure and large pores of cotton fiber mats give rise to a low normalized pressure drop. The high
filtration performance results from the unique protein morphology on the cotton fiber surface, e.g. homo-
geneously distributed protein particles via denaturation process, creating an optimized surface area for inter-
actions between protein and pollutants. In addition, to enhance the filtration efficiency for capturing fine par-
ticulate pollutants (i.e. PM1.0, PM0.3), a synergistic bi-layered air filter which combines the zein-functionalized
cotton fibers with a thin layer of protein nanofibers is fabricated. It is further demonstrated that the unique
configuration of the composite air filter at the upstream side for airflow and protein nanofiber at the downstream
side leads to remarkable filtration efficiencies over 99.0% for PM of a broad range of sizes due to a synergistic
effect. This study provides a new and cost-effective method with a “green” solvent involved for efficiently
fabricating “green” and efficient air filters by combining microfibers and nanofibers.

1. Introduction
Indoor air quality is not only affected by the polluted air outside but
also by indoor pollution. As people usually spend more time inside
relatively enclosed spaces/buildings, cleaning indoor air is more and
more important for a human’s health, in particular toxic chemicals such
as formaldehyde (HCHO) and carbon monoxide are concerning (CO)
[1–4]. Indoor air quality is getting worse due to the increasingly serious
atmospheric pollution. Major pollutants in the air consist of particlulate
matter (PM) pollutants resulting from various human and industrial
activities, e.g. the intense burning of fossil fuel [5]. These PM pollu-
tants, with a wide range of diameters, are also threatening individuals’
health [6,7]. Furthermore, some PM pollutants with small particle sizes
and large surface area may be highly reactive under direct sunlight [8].
As a result, more species of toxic particles can be produced by complex
reactions. Therefore, multifunctional air filters that can efficiently
capture more species of pollutants are critical.
As a result of pollution threats, various air filters have been pro-
duced. The two major categories of commercial air filters are high-ef-
ficiency particulate air (HEPA) filters and activated carbon filters.
HEPA, which is primarily made of glass fibers or synthetic polymer fi-
bers such as polyethylene (PE) and polypropylene (PP), can efficiently
remove most PM pollutants. The major mechanisms of HEPA are im-
pact, interception, and diffusion [9]. However, HEPA filter cannot
capture toxic chemicals since there are not functional groups present in
the fiber structures. Meanwhile, activated carbon filters and specially
functional filters can efficiently absorb toxic chemicals, but have lower
filtration efficiency for PM [10–12]. In addition, some new filters ad-
dress increasing efficiency for removing PM pollutants or toxic chemi-
cals have also been studied. For instance, titanium dioxide-based filters
with different crystal structures can effectively catalyze the decom-
position of HCHO [13,14]. Moreover, filters made of electrospun
polymeric fibers have shown excellent filtration efficiency for PM
[15,16]. However, these filters are not only costly to produce in terms

⁎
Corresponding authors.
E-mail addresses: xuewei.fu@wsu.edu (X. Fu), katie_zhong@wsu.edu (W.-H. Zhong).

https://doi.org/10.1016/j.seppur.2019.115837
Received 17 April 2019; Received in revised form 19 July 2019; Accepted 19 July 2019
Available online 20 July 2019
1383-5866/ © 2019 Elsevier B.V. All rights reserved.
J. Liu, et al.
of raw materials and fabrication procedures but are also potentially
hazardous to the environment at their disposal. Therefore, developing
cost-effective bio-based filters which have high filtration capabilities for
both PM and gaseous chemicals will be a significant development.
To enable capabilities of capturing both PM and gaseous chemicals
simultaneously and improve environmental friendliness of the resulting
filters, exploiting natural biomass, such as various protein, to fabricate
air filters is one of the most promising methods. It has been reported
that the protein-based filters consisting of gelatin, silk, zein or soybean
protein nanofibers, can not only filter out PM but also toxic chemicals
[17–22]. Utilizing protein nanofibers to fabricate air filters has im-
portant advantages. For instance, protein nanofibers have a huge sur-
face area and high surface energy facilitating the interaction/trapping
of more PM pollutants. In addition, the protein nanofibers may absorb
gaseous chemicals efficiently due to a huge number of functional groups
in the protein’s chemical structures. It is known that the basic building
blocks of protein include 20 different amino acids; these numerous
functional groups provide protein-gaseous chemical interactions.
However, achieving protein nanofibers heavily relies on electrospin-
ning technology; the productivity of electrospinning is not high enough
to make protein nanofibers commercial [17–20]. In addition, the filters
consisting of large amounts of electrospun protein nanofibers have
several issues. One of the critical issues is their relatively high pressure
drop. For instance, the pressure drop of a functional protein-based
nanofibrous filter with areal density of 3.80 g/m2 reached over 200 Pa
[17]. Although lowering the pressure drop by decreasing the active
ingredient, or the protein nanofibers, is possible, it compromises the
filtration capacity and efficiency of the filters. Hence, it is crucial to find
a method for not only minimizing the negative effects of electrospin-
ning on air pressure drop of the protein-based filter but also maintain
the advantages of protein. To achieve this, combining plant fibers
functionalized by protein via a simpler method with a minimal amount
of electrospun nanofibers can be a suitable strategy.
Evaporation-controlled assembly is a traditional, widely used and
cost-efficient method for grafting nanostructures on fiber frames. For
example, through evaporation approaches, attaching protein nanos-
tructures on cellulose fibers has been achieved [23–27]. However,
fabricating protein-based air filters via evaporation-controlled assembly
is rarely reported. While exploiting evaporation-controlled assembly to
fabricate cellulose-based protein air filter, the filtration performance
may heavily depend on the selection of solvents for denaturing protein.
This dependence is due to the fact that the solvent may determine the
surface morphology of the protein on cellulose fiber [28–33]. More-
over, a suitable solvent should be environmental-friendly during the
fabrication. Lastly, the fabrication process should be simplified since a
simple procedure may also save energy. Previously, we fabricated a
filter by exploiting wood pulp as a frame to hold whey/bacterial cel-
lulose nanoparticles [34]. Although the resulting cellulose-based filters
with protein nanostructures have excellent performance, the fabrication
procedure has some issues. These issues include the utilization of acidic
solvent (acetic acid) and the complexity of the fabrication. In total,
application of simple and “green” solvents for effectively denaturing
protein is the critical factor for low-cost fabrication of the bio-filters.
In this study, we design and fabricate a bi-layered air filter made of
zein (corn protein) functionalized cotton fibers (Z-CoF) and a very low
amount of electrospun zein nanofibers (ZNF). The Z-CoF is functiona-
lized by the protein via a subtly controlled evaporation assembly pro-
cess, such that a homogeneous growth of zein particles can be achieved
on the fiber surface. The grafted protein particles significantly improve
the PM2.5 filtration efficiency to 91.4%, as compared with the native
cotton-fiber (70.3%). Moreover, the bi-layered air filter with a config-
uration of Z-CoF at the upstream and ZNF at the downstream side of the
airflow, further improves filtering of fine PM pollutants. An extremely
low pressure-drop and high filtration efficiency are achieved: 99.0% for
PM2.5 and 93.3% for PM0.3 with only 112.5 Pa/g; meanwhile, such bi-
layered air filter shows effective capture of chemical gases such as
2
Separation and Purification Technology 229 (2019) 115837
carbon monoxide (CO) and formaldehyde (HCHO) as well.
2. Materials and methods
2.1. Fabrication of bi-layered air filter
2.1.1. Materials
Zein protein (α-zein, 95% purity) was purchased from Sigma-
Aldrich Co. Ltd. The cotton fiber was purchased from WinCo Foods, Inc
(Fig. S1a, Supplementary Material). Plastic meshes were purchased
from Pullman Building Supply, a local provider (Fig. S1b,
Supplementary Material). 1-Butanol (99.9% purity) was purchased
from J.T. Baker, while acetone (99.9% purity) and ethanol (99.9%
purity) were purchased from Koptec and Macron Co. Ltd. All materials
and chemicals were used as received without further treatments.
2.1.2. Fabrication of functionalized cotton-fiber (CoF)
Zein solutions were prepared by dissolving zein protein in three
varieties of solvents: (1) acetone solution (70 wt% acetone, 30 wt%
deionized (DI) water), (2) ethanol solution (70 wt% ethanol, 30 wt% DI
water) and (3) ternary solvent (50 wt% acetone, 25 wt% 1-Butanol and
25 wt% DI water). All of the solutions were prepared at room tem-
perature (25 °C) and the concentration of zein protein was fixed to be
0.50 wt%. To fabricate zein-functionalized CoFs (Z-CoFs) by different
solvents, CoFs were soaked in the three zein solutions individually for
30 min at 25 °C allowing the adsorption of zein solution by CoFs.
Subsequently, the wet CoFs were transferred to a gravity convection
oven to evaporate the solvents at 50 °C for 2.5 h. To study the effects of
zein concentration on the filter properties, a group of zein/ethanol
aqueous solution with different zein concentrations including 0.25 wt
%, 0.50 wt% 0.75 wt% and 1.00 wt% was prepared at 25 °C. Then, CoFs
were soaked in these solutions individually for 30 min at 25 °C. The wet
CoFs were dried in a gravity convection oven for 2.5 h at 50 °C. To study
the effects of evaporation temperature on the filter properties, a group
of Z-CoFs were prepared by soaking CoFs in zein/ethanol aqueous so-
lution with a zein concentration of 0.75 wt% for 30 min at 25 °C. Then,
the wet CoFs were dried at 25 °C for 24 h and at 40 °C, 50 °C, 60 °C for
2.5 h, respectively.
2.1.3. Fabrication of zein nanofiber (ZNF) and the synergistic bi-layered air
filter
ZNF was fabricated by electrospinning as reported in our previous
study [19]. The precursor solution was prepared by dissolving zein in
the ternary solvent as introduced above. The protein concentration of
this solution was 25 wt%. The fabrication was continued in an elec-
trospinner (Nanospinner 24, Inovenso) at 25 °C, and plastic mesh was
used as the substrate. The flow rate of the solution was 2.0 ml/h; the
fabricating voltage was 17.5 kV, and the distance between the mesh and
nozzle was fixed to be 15 cm. The fabrication time was fixed to be only
3.5 min. To fabricate the bi-layered air filters, ZNF and Z-CoF were
pressed together in our sample holder for the filtration performance
test. The two configurations of these two components were dependent
on which of them located at the upstream side of the airflow.
2.2. Characterizations
2.2.1. Morphology and composition
The protein particle size in the solvents was studied via dynamic
laser light scattering (Zetasizer Nano, Malvern Instruments). Zein pro-
tein in ternary solvent, acetone aqueous and ethanol aqueous solution
were analyzed in this study. The surface morphology of all the samples,
including Z-CoFs and ZNF, was investigated by using scanning electron
microscopy (SEM, FEI SEM Quanta 200F). The surface contact angle of
protein films was studied by a contact angle analyzer (OCA 15 plus
instrument and SCA 20 software). The zein films for the contact angle
analysis were prepared by casting the three solution (zein in ternary
J. Liu, et al.
solvent, acetone aqueous and ethanol aqueous) on aluminum foil and
then heat evaporating at 50 °C.
2.2.2. Air filtration testing
The concentrated polluted air sample containing a wide range of PM
pollutants, HCHO, and CO was produced by burning joss sticks. To
adjust the concentration of these pollutants, the polluted air sample was
then diluted in a glass bottle to a measurable level for a particle counter
(CEM DT-9881), a formaldehyde meter (Omega, HHAQ-108) and a
carbon monoxide meter (Sensorcon, INS-CO-01). Moreover, the pres-
sure drop was measured by utilizing a manometer (UEi, EM201-B),
while the airflow rate was maintained in 4 L/min. The filtration effi-
ciency (η) of PMs, HCHO and CO was defined by Eq. (1):
η = (Cp − Cc )/ Cp
where Cp and Cc are the air pollutant concentration before and after the
filtration experiment.[35] To minimize the effect of the filter’s weight
to raw pressure drop, normalized pressure drop (norm. pressure drop)
has been involved.[34] norm. pressure drop is defined by Eq. (2):
norm . pressure drop = ΔP / m
where ΔP is the raw pressure drop and m is the mass of the sample.
Thus, the unit of norm. pressure drop is Pa/g.
The areal density is defined by Eq. (3):
AD = m / S
where m and S are the weight of protein on the filter and square meter
of the filter.
3. Results and discussion
Herein a synergistic all-biomass air filter is proposed and fabricated
via constructing a bi-layered structure with zein-functionalized cotton
fiber (Z-CoF) at the top and a low amount of zein nanofiber (ZNF) at the
bottom. The unique configuration of this bi-layered air filter brings
about synergistic effects for improving the capability of capturing
various pollutants of broad sizes while maintaining a relatively low
pressure drop. Specifically, as illustrated in Fig. 1, native zein protein
comprises 20 different types of amino acids and possesses quaternary
structure by strong intermolecular interactions, i.e. ionic interaction, H-
bonding, disulfide bridge, etc. Denaturation of zein disrupts most of the
Fig. 1. Illustration of fabrication process of a synergistic bi-layered air filter via combining cotton fiber (CoF) (at the top) and zein nanofiber (ZNF) (at the bottom).
Separation and Purification Technology 229 (2019) 115837
intermolecular interactions and significantly reduces the particle size of
zein, such that the functional groups of zein can be exposed and further
utilized. The exposed functional groups of zein are demonstrated to
have strong interactions with various pollutants, e.g. PM, chemical
gases, as reported by previous studies [17–19,34]. Cotton fiber (CoF) is
a class of natural microfibers with very loose fibrous structure and good
mechanical properties. These advantages make CoF an appropriate
skeleton which provides low pressure drop and mechanical support.
Based on these considerations, we functionalize CoF with zein through
a subtly controlled evaporation process to form uniformly distributed
zein nanoparticles on the surface of CoF. The zein-functionalized CoF
(Z-CoF) shows significantly improved filtration capability and low
pressure drop even with extremely high areal density. Additionally, to
further enhance the filtration capability, a synergistic bi-layered filter is
(1) constructed by adding a small amount of zein nanofiber (ZNF) at the
bottom side of Z-CoF. The bi-layered air filter provides two advantages
for enhancing filtration performance. Firstly, Z-CoF and ZNF act as the
“double-insurance” for capturing most of the pollutants. Secondly, Z-
CoF regulates the airflow and improves the performance of ZNF for
capturing fine PM pollutants (PM0.3-PM1.0). Both of the two advantages
(2) will be discussed in detail later.
In this study, we propose an evaporation-controlled assembly
strategy for functionalizing CoF by denatured zein particles. It is well
known that solvents play a critical role in the denaturation of zein and
the morphology control of denatured zein particles. More importantly,
(3) during evaporation process, solvents significantly affect the interaction
between zein and CoF. Therefore, they are the major influences for the
evolution of denatured zein particle on the surface of CoF. We adopt
three types of solvents, aqueous acetone (aq. acetone), aqueous ethanol
(aq. ethanol) and ternary solvent (mixture of acetone, butanol and
deionized water), for denaturing zein (the details of the composition of
solvents can be found in Experimental section). It can be seen in Fig. 2a
that the ternary solvent presents the strongest ability to denature zein
among the three solvents, indicated by the smallest particle size of
denatured zein (ca. 248 nm), which is consistent with the previous
study [19]. On the contrary, aq. acetone shows the poorest denatura-
tion capability with the largest zein particle size of ca. 645 nm; and aq.
ethanol sets in the middle (particle size of denatured zein: ca. 378 nm).
Surprisingly, it is found that the surface properties of zein are
greatly tuned by the solvents. As shown in Fig. 2b, the contact angles of
a water droplet on the zein solid films denatured in different solvents
3
J. Liu, et al. Separation and Purification Technology 229 (2019) 115837

Fig. 2. Morphological studies of zein protein denatured in different solvents and the resulting zein-functionalized cotton-fiber (Z-CoF). (a) Particle size of zein
denatured in different solvents. (b) Water contact angle of zein films by different solvents. (c) SEM images of raw CoF. (d)–(f) SEM images and schematic of the
interactions between denatured zein particles and CoF in (d) ternary solution, (e) aqueous acetone solution and (f) aqueous ethanol solution.

decrease in sequence of ternary solvent (81.5°), aq. acetone (69.1°) and zein to exhibit the most hydrophilicity. The surface properties of de-
aq. ethanol (55.0°). This indicates that the zein particles denatured in natured zein particles are affected by the polarity of the solvents [33].
ternary solvent and aq. acetone are far less hydrophilic than in aq. As acetone (relative polarity: 0.355) and 1-butanol (relative polarity:
ethanol. In other words, among the three solvents, aq. ethanol causes 0.586) possess much lower polarity as compared with ethanol (relative

4
J. Liu, et al.
polarity: 0.654), in ternary solvent or aq. acetone, zein molecules tend
to bind the acetone/butanol molecules via nonpolar-nonpolar interac-
tions. During evaporation process, the nonpolar part of the zein mole-
cules are attracted by the solvent molecules making the zein film sur-
face comparatively less hydrophilic. On the contrary, in aq. ethanol, the
relatively strong interaction between the polar part of zein and the
ethanol molecules. This interaction results in the increased hydro-
philicity of zein.
The surface morphology of raw CoF and Z-CoFs prepared from the
three zein solutions were investigated; and the SEM images are shown
in Fig. 2c–f. As shown in Fig. 2c, the raw CoF presents a ribbon-like
fibrous structure with wrinkles on the surface, the diameter of which is
20–40 μm. The functionalization of CoF by zein dramatically changes
the microstructure of CoF. As shown in Fig. 2d, films are formed on the
surface of Z-CoF while treating CoF with zein denatured in ternary
solvent (abbreviated as Z/Ter-CoF). Regarding the zein/aq. acetone
solution treated Z-CoF (abbreviated as Z/Ace-CoF) as shown in Fig. 2e,
both single and aggregated zein particles can be observed, which results
in a very non-uniform distribution of the denatured protein particles.
However, zein/aq. ethanol solution treated Z-CoF (abbreviated as Z/
Eth-CoF) shows a homogeneous distribution of denatured zein particles
on the surface of individual fiber without forming aggregates in Fig. 2f.
The above morphological studies reveal distinctly different micro-
structure features of Z-CoFs treated by three solvents, which result from
the different particle size and surface property of the denatured zein
particles. As depicted in Fig. 2d, in ternary solvent, denatured zein
particles present relatively less hydrophilic surface leading to poor in-
teractions between zein and cotton fiber with highly hydrophilic sur-
face due to its rich hydroxyl groups. As a result, the strong inter-
molecular interaction of the well-denatured small zein particles make
them uniformly form the films during evaporation. In the case of zein/
aq. acetone solution as shown in Fig. 2e, although the interaction be-
tween denatured zein particles and CoF might be stronger than that of
zein/ternary solution and CoF, the poorly denatured zein particles tend
to agglomerate and form large clusters. In contrast, denatured zein
particles in aq. ethanol exhibit the most hydrophilic surface in this
study, giving rise to strong hydrophilic interactions between zein and
cotton (see Fig. 2f). Therefore, denatured zein particles are well dis-
tributed on the surface of CoF instead of forming large agglomerates or
films.
To evaluate the air filtration performance, PM2.5 filtration efficiency
and normalized pressure drop (pressure drop/areal density, abbre-
viated as norm. pressure drop) of the raw CoF filter and all three Z-CoF
filters are examined. As shown in Fig. 3a, the PM2.5 filtration efficiency
of the raw CoF filter is 70.3%; and the norm. pressure drop of it is
114.8 Pa/g, which is the lowest one among all the samples. This fil-
tration performance benefits from the fluffy fiber structure and polar
surface property of CoF, enabling some filtration of pollutants and low
pressure drop. It is noted that all Z-CoF filters show much higher PM2.5
filtration efficiencies and norm. pressure drops compared with CoF. In
specific, Z/Eth-CoF filter reveals the highest PM2.5 filtration efficiency
of 91.4% and the lowest norm. pressure drop of 139.4 Pa/g among the
three types of Z-CoF filters. These results indicate that the denatured
zein particles grown on the CoF surface substantially improve the air
filtration performance; and the morphologies of them play an important
role in the filtration performance. To further investigate the influence of
surface morphology on the filtration performance of Z-CoF filters, the
diameter distribution of denatured zein particles on the surface of Z/
Ace-CoF and Z/Eth-CoF is investigated. The diameter distribution of Z/
Ter-CoF cannot be provided due to the formation of films. As shown in
Fig. 3b, there is a noticeable diameter difference between the denatured
zein particles on the surface of Z/Ace-CoF and Z/Eth-CoF (ca. 831 nm
vs ca. 643 nm). Since the denatured zein on the surface of Z/Ace-CoF
also exhibits significant aggregation, the denatured protein in this
sample possesses much lower surface area compared with that of Z/
Eth-CoF. The filtration mechanisms for removing PM pollutants by the
5
Separation and Purification Technology 229 (2019) 115837
three filters are proposed in Fig. 3c. Based on the previous studies, as a
result of various functional groups within amino acids, strong interac-
tions between denatured zein and particulate pollutants can be pro-
vided, such as dipole-dipole interaction [20,36]. The interactions are
beneficial for removing the PM pollutants from the air [35,37]. How-
ever, all these interactions are affected by the morphologies of zein.
Observed in Z/Ter-CoF filter, the film structures, which wrapped and
covered some pores of CoF, improve the filtration efficiency since the
filled pores become effectively physical traps for the pollutants. How-
ever, the covered pores substantially increase the norm. pressure drop
(168.3 Pa/g). In the case of Z/Ace-CoF filter, the aggregated zein par-
ticles reduce the surface area of the exposed protein. The reduced
surface area greatly decreases the probability of pollutants impacting
the fiber surface, resulting in lower filtration efficiency. On the con-
trary, for Z/Eth-CoF filter, the uniformly distributed zein particles ef-
fectively increase the surface area of zein and the interactions between
denatured zein and pollutants. Consequently, it delivers the highest
filtration performance while maintaining the lowest norm. pressure
drop of the three Z-CoF air filters.
The above studies indicate that zein/aq. ethanol solution treated
CoF presents the highest filtration performance. To optimize the mi-
crostructures of denatured zein particles on the surface of CoF and
enhance the filtration performance of the resulting filters, we in-
vestigate the evaporation-controlled assembly process by adjusting the
concentration of zein in aq. ethanol and evaporation temperature. It is
found that a homogeneous distribution of the denatured zein particles
can only be achieved with an appropriate evaporation temperature and
concentration of zein in the solvent. Fig. 4a shows the SEM image of Z-
CoF treated by 0.75 wt% zein solution and evaporated the solvent at
25 °C. One can easily observe that denatured zein exhibits severe ag-
gregation behavior leading to the formation of protein agglomerates
and films which wrap around the fibers. Then, with the increased
evaporation temperature (40 °C, Fig. S2a, Supplementary Material), the
particle size of denatured zein on the surface of Z-CoF decreases gra-
dually (ca. 725 nm). After that, as shown in Fig. 4b, while increasing the
temperature to 50 °C for removing the solvent from the Z-CoF treated
by 0.75 wt% zein solution, denatured zein particles are homogeneously
distributed on the surface of CoF with an average particle size of
589 nm. Eventually, while evaporating the solvent at 60 °C (Fig. S2b,
Supplementary Material), the denatured zein particles maintain a si-
milar size as that assembled at 50 °C. This indicates that a higher eva-
poration temperature leads to a higher evaporation rate. The increased
evaporation rate significantly contributes to the formation of in-
dividualized zein particles and effectively prevents the re-agglomera-
tion of them in the drying process. However, if the zein concentration in
the solution is increased to 1.00 wt%, as shown in Fig. 4c, the high
evaporation temperature (i.e. 50 °C) cannot prevent the re-agglomera-
tion of the denatured protein particles. The concentrated zein solution
results in formation of films due to the oversaturation of protein during
evaporation. Meanwhile, if treated CoF by 0.25 wt% of zein solution
and evaporated it at 50 °C (Fig. S2c, Supplementary Material), although
the denatured protein particles can be found on the surface of resulting
Z-CoF, the areal density of the protein in the sample is only 2.08 g/m2
(Fig. S3). It is far lower than in Z-CoF filters fabricated by 0.50 wt%
solution (8.69 g/m2) and 0.75 wt% solution (12.52 g/m2). This low
areal density indicates that the denatured zein particles may not be
enough to fully functionalize the Z-CoF filter. In a nutshell, two im-
portant points are worthy of discussion. Firstly, temperature is a deci-
sive factor affecting the evaporation rate of solvents. A low evaporation
temperature, such as 25 °C, causes the aggregation behavior of the
denatured zein particles. Nonetheless, the agglomeration of denatured
zein is alleviated with a much higher evaporation temperature, such as
50 °C, since the faster drying process helps to maintain the original state
of the denatured protein particles in solution. Secondly, with the in-
crease of zein concentration, the aggregation is unavoidable. This is
because with a higher zein concentration, the denatured protein may
J. Liu, et al.
Fig. 3. PM2.5 filtration performance of Z-CoFs by different solvents as compared with pristine CoF. (a) Removal efficiency and pressure drop of different Z-CoFs as
compared with CoF. (b) Diameter distribution of denatured zein particles on the surface of Z/Ace-CoF and Z/Eth-CoF (c) Schematic illustration of effects of solvents
on the PM2.5 filtration performance of Z-CoF filters.
become oversaturated during evaporation, resulting in the re-aggrega-
tion behavior.
The evaporation conditions also influence the air filtration perfor-
mance of Z-CoF filters. We first investigate the relationship between the
concentration of zein solution and the filtration performance of the
resulting Z-CoF filters (the evaporation temperature is fixed at 50 °C) as
shown in Fig. 4d. When treating CoF with 0.25 wt% zein solution, the
PM2.5 filtration efficiency of Z-CoF filter slightly increases from 70.3%
for raw CoF filter to 74.9%, due to the scarce loading of denatured
protein (2.08 g/m2, Fig. S3, Supplementary Material). Meanwhile, the
Z-CoF filter prepared from 0.75 wt% zein solution shows a similar PM2.5
filtration efficiency of 90.4% with the 0.50 wt% Z-CoF filter (91.4%).
However, increasing the protein concentration to 1.00 wt% deteriorates
the filtration efficiency of Z-CoF filter to 78.0%. Moreover, although all
the Z-CoF filters show higher norm. pressure drops than that of the raw
CoF filter (114.8 Pa/g), Z-CoF filters fabricated by 0.25 wt%, 0.50 wt%
and 0.75 wt% zein solutions present comparative norm. pressure drops
(120–140 Pa/g). In contrast, the norm. pressure drop of Z-CoF filter
produced by 1.00 wt% zein solution significantly increases to 280.1 Pa/
g due to the formation of protein films blocking the pores. Since the Z-
CoF filter made of 0.75 wt% zein solution presents better sample uni-
formity than that of 0.50 wt% Z-CoF (see Fig. S3, Supplementary
Material) and exhibits comparable air filtration performance and norm.
pressure drop, 0.75 wt% zein solution are adopted to fabricate Z-CoF for
subsequent studies.
Fig. 4e shows the effect of evaporation temperature on the filtration
performance of Z-CoF filters (the concentration of zein solution for
6
Separation and Purification Technology 229 (2019) 115837
treating CoF is fixed at 0.75 wt%). It is found that by increasing the
evaporation temperature from 25 to 60 °C, the pressure drops of all the
Z-CoF filters are similar in the range of 135–140 Pa/g. However, the
PM2.5 filtration efficiency constantly increases from 81.1% to 90.8%.
Fabricating with elevated temperature, the homogeneously distributed
denatured zein particles on the surface of the filters are responsible for
the strong capability of capturing pollutants. Also, the filtration effi-
ciency of the Z-CoF filter evaporated the solvent at 50 °C is very com-
parative with the case of 60 °C (90.4% vs 90.8%). In the basis of above
studies, it is considered that with 0.75 wt% zein solution and eva-
poration temperature of 50 °C (more energy efficient), the morphology
of denatured zein particles on the surface of Z-CoF filter can be opti-
mized to deliver the highest air filtration performance.
In addition, the chemical absorption performance of the Z-CoF filter
treated by 0.75 wt% zein solution and evaporated solvent at 50 °C is
investigated and compared with untreated CoF. The toxic gaseous
chemicals include formaldehyde (HCHO) and carbon monoxide (CO).
As shown in Fig. 4f, the native CoF filter only absorbs 38.4% HCHO and
9.0% CO, possibly because of CoF has plenty of hydroxyl groups on the
surface that may attract HCHO. However, it is worth noting that Z-CoF
filter absorbs 61.7% HCHO and 26.1% CO, which are much higher than
in CoF filter. The functional groups in protein provide strong attraction
to gaseous chemicals, including polar-polar interaction and hydrogen
bonding [19,20]. In addition, the large surface area of the denatured
zein particles rested on the fiber surface enhances the adsorption of
HCHO and CO.
Although Z-CoF air filters is efficient at removing PM2.5 pollutants
J. Liu, et al.
from the air, a low amount of zein nanofiber (ZNF) is introduced to help
remove PM0.3 to PM1.0 pollutants. This is because the fine particulates
are even more hazardous to individuals’ health [6]. As shown in the
SEM image in Fig. 5a, zein nanofiber fabricated by electrospinning
exhibits a ribbon-like fibrous structure. This distinctive structure pro-
vides two advantages: high PM-capturing efficiency and relatively low
pressure drop [19]. However, according to our previous study [19], to
achieve desired filtration performance, the areal density of ZNF must
reach about 12 g/m2, giving rise to an extremely high norm. pressure
drop of 4148 Pa/g. To address this issue, we combine a thin layer of
ZNF with Z-CoF as illustrated in Fig. 5a, which results in bi-layered air
filters with two configurations: (1) ZNF/Z-CoF filter with ZNF located at
the upstream of airflow; (2) Z-CoF/ZNF filter with Z-CoF located at the
upstream of airflow. As displayed in Fig. 5b, the thin layer of ZNF filter
possesses a very low areal density (2.31 g/m2); and the norm. pressure
drop of the filter is only 165 Pa/g in comparison of our previous study
(4148 Pa/g) [19]. PM2.5 removal efficiency of ZNF filter is corre-
spondingly deteriorated from 99.9% to 88.2%. It is revealed that by
combining ZNF and Z-CoF, the bi-layered air filters exhibit much better
PM2.5 filtration performance than that of ZNF filter or Z-CoF filter in-
dividually. More significantly, Z-CoF/ZNF filter shows even higher
PM2.5 filtration efficiency of 99.0% than that of ZNF/Z-CoF filter
(93.2%). Furthermore, the norm. pressure drops of the two bi-layered
7
Separation and Purification Technology 229 (2019) 115837
Fig. 4. Morphological studies and air filtration
performance of Z-CoF (Z/Eth-CoF) fabricated by
different concentrations of zein/aq. ethanol so-
lution and evaporation temperatures. (a)–(c)
SEM images of Z-CoF fabricated with different
concentrations of zein solution and evaporation
temperatures: (a) 0.75 wt%, 25 °C, (b) 0.75 wt%,
50 °C and (c) 1.00 wt%, 50 °C, respectively. (d)
Relationship between zein solution concentra-
tion and air filtration performance of Z-CoF air
filter fabricated with evaporation temperature of
50 °C. (e) Relationship between evaporation
temperature and air filtration performance of Z-
CoF air filter fabricated with 0.75 wt% zein so-
lution. (f) Chemical filtration efficiency of raw
CoF and Z-CoF filter fabricated with 0.75 wt%
zein solution and evaporation temperature of
50 °C.
filters (around 112.5 Pa/g) is much lower than in their components
(ZNF filter: 165.0 Pa/g, Z-CoF filter: 139.4 Pa/g).
The air filtration performance of the two bi-layered filters, ZNF, Z-
CoF, and raw CoF filters for removing PM pollutants with a wide range
of diameter (from 0.3 to 2.5 μm) is shown in Fig. 5c. One can notice that
CoF filter shows the lowest air filtration performance throughout the
tested PM range, due to the innate surface properties of CoF. More
significantly, the efficiency of Z-CoF/ZNF filter for removing all sizes of
PM pollutants is remarkably higher than in ZNF, Z-CoF and even ZNF/
Z-CoF filters. Namely, the air filtration efficiencies of Z-CoF/ZNF for
PM0.3, PM0.5, PM1.0, and PM2.5 are 93.3%, 98.2%, 98.7%, and 99.0%,
respectively. In contrast, the ZNF/Z-CoF filter shows only slightly better
air filtration performance than in ZNF and Z-CoF filters. Furthermore,
the chemical filtration performance is examined and shown in Fig. 5d.
HCHO filtration efficiencies of ZNF, ZNF/Z-CoF and Z-CoF/ZNF filters
are 55.4%, 62.5% and 66.2%; and CO filtration efficiencies are 22.1%,
27.0% and 26.6%, respectively. This result indicates that, compared to
the individual components (ZNF and Z-CoF filters), the bi-layered air
filters deliver higher chemical filtration efficiencies. In specific, the
HCHO filtration efficiency of Z-CoF/ZNF filter is much higher than that
of ZNF/Z-CoF filter. However, CO filtration efficiency of ZNF/Z-CoF
and Z-CoF/ZNF filters are almost identical. This is because CO is a re-
latively stable molecule (CO and nitrogen are isoelectronic sharing
J. Liu, et al.
Fig. 5. Air filtration performance of a bi-layered air filter. (a) Configuration of ZNF/Z-CoF and Z-CoF/ZNF air filters, and morphology of zein nanofiber (ZNF). (b) Air
filtration performance of two bi-layered air filter with different configurations, as compared with ZNF. (c) PM filtration efficiency of various air filters. (d) Chemical
filtration efficiency of two bi-layered air filter with different configurations, as compared with ZNF.
some similar properties), indicating that its interaction with denatured
protein might be poorer than that of HCHO. The abovementioned re-
sults suggest that the bi-layered filters present much better filtration
performance, as compared with the individual components: ZNF and Z-
CoF filters. More importantly, the configuration of the bi-layered air
filters plays a vital role in the air filtration performance, which will be
discussed in detail below.
To investigate how the bi-layered configuration contributes to the
filtration, we observe the upstream and downstream sides of the ZNF
filters after filtration testing for the two bi-layered filters as shown in
Fig. 6a, b. In Fig. 6c for ZNF/Z-CoF filter, the captured pollutants can be
rarely found at both sides of ZNF filter. In contrast, for the case of Z-
CoF/ZNF filter, many pollutants are captured by the nanofibers in up-
stream side of ZNF filter, while the downstream side is absent of pol-
lutants as shown in Fig. 6d. To elucidate the effects of air filter con-
figuration on the air filtration performance, the possible models are
depicted in Fig. 6e, f. The components of the bi-layered air filters pre-
sent different porous structures, i.e. ZNF filter with nanofibrous struc-
ture and Z-CoF filter with microfibrous structure. This leads to a dif-
ference of airflow velocity between the two layers for both bi-layered
air filters. In specific, for the ZNF/Z-CoF filter in Fig. 6e, when airflow
passes through ZNF filter first, it significantly accelerates the airflow
due to its tight porous structure with extremely small pores [38].
Meanwhile, it is found that the pollutants are only trapped by the up-
stream surface of ZNF filter. As a result, the filtration ability of the latter
layer, Z-CoF filter, is decreased, which can be proved by the fact that
the filtration performances of ZNF and ZNF/Z-CoF filters are similar
(see Fig. 5c). In other words, in the ZNF/Z-CoF filter, the filtration of
pollutants can be attributed to the ZNF filter. By contrast, for the Z-CoF/
ZNF filter shown in Fig. 6f, the loose porous structure and relatively
large pore size of Z-CoF filter make little contribution to accelerate the
airflow. Consequently, acted as “double-insurance”, both Z-CoF and
ZNF filters capture pollutants simultaneously as indicated by the SEM
images in Fig. 6d.
8
Separation and Purification Technology 229 (2019) 115837
4. Conclusion
In this study, we reported an evaporation-controlled strategy for
fabricating a zein protein-functionalized cotton fiber (Z-CoF) air filter
capable of effectively capturing PM2.5 and chemical gases. It is revealed
that only with an appropriate solvent (ethanol aq. solution), an opti-
mized evaporation temperature (50 °C) and concentration of zein so-
lution (0.75 wt%), a homogeneous growth of well dispersed zein par-
ticles on the surface of cotton-fibers can be achieved. As a result, a loose
fibrous structure of zein-functionalized cotton fibers with sufficient
interactions between protein and pollutants show significant improve-
ment in filtration efficiency while maintaining a low norm. pressure
drop in the Z-CoF air filter. Furthermore, synergistic bi-layered air fil-
ters via combining a thin layer of zein nanofiber and Z-CoF with two
configurations are demonstrated to further improve the filtration effi-
ciency especially for fine particles. It is found that this unique config-
uration: Z-CoF at the upstream and zein nanofiber (ZNF) at the down-
stream, delivers remarkably higher filtration efficiencies, i.e. above
99% for PM with broad sizes and lower norm. pressure drop of ca.
112.5 Pa/g, as compared with the two individual components.
Moreover, a significant chemical filtration efficiency is also observed,
i.e. 66.2% of formaldehyde (HCHO). The mechanism on the synergic
effect of Z-CoF and ZNF is analyzed. This study demonstrates that the
evaporation-controlled approach is a cost-effective protein-functiona-
lization strategy for fabricating composite air filters and lay an im-
portant foundation for designing and constructing advanced multi-
layered air filters.
Acknowledgments
This work was financially supported by Washington State University
Office of Commercialization and Washington Research Foundation. The
authors appreciate the School of Biological Sciences Franceschi
Microscopy & Imaging Center (FMIC) at Washington State University
for providing the field emission electron microscope.
J. Liu, et al.
Fig. 6. Contribution of bi-layered configuration to air filtration. (a)–(b) Configuration of (a) ZNF/Z-CoF and (b) Z-CoF/ZNF air filters. (c)–(d) SEM images of
upstream and downstream of ZNF in (c) ZNF/Z-CoF and (d) Z-CoF/ZNF air filters after filtration testing. Scale bar: 10 μm. (e)–(f) Illustration of air filtration situations
in (e) ZNF/Z-CoF and (f) Z-CoF/ZNF air filters.
Appendix A. Supplementary material
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.seppur.2019.115837.
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