NanoImpact 19 (2020) 100240

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NanoImpact
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Research paper

Advanced filtration and lung deposition models of airborne multi-walled T

carbon nanotubes for inhalation exposure assessment
⁎
Tobias Hammera,b, Panagiota Sachinidoua,b, Xu Hec, Zhengyuan Pana,b, Yeon Kyoung Bahka,b,
a
Institute of Environmental Engineering, ETH Zurich, 8093 Zurich, Switzerland
b
Advanced Analytical Technologies laboratory, Empa, 8600 Dübendorf, Switzerland
c
State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, 150090, China

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

Editor: Philip Demokritou Precise prediction of airborne carbon nanotube (CNT) filtration and deposition in the lung is of significant
Keywords: importance to find proper control media and to perform exposure assessment to quantify the toxicity for emitted
Carbon nanotube airborne CNTs. We executed a systematic study in order to evaluate the inhalation exposure of inhaled single
Agglomerate mixing state standing airborne multi-walled carbon nanotubes (MWCNTs) and CNT agglomerates, by assessing their filtration
Agglomerated fibrous particle and deposition in the deep lung using calculation models. Filtration, inhalation and deposition were influenced
Filtration model by the agglomeration of the fibrous particles and by the agglomerate mixing state. We revised previous models
Lung deposition model and developed the models for realistic CNT mixtures in air with a new approach using the mixing states of CNT
agglomerates and single standing CNTs. We verified our newly developed filtration model empirically. The
calculated lung deposition for the realistic CNT mixtures and CNT agglomerates showed much higher deposition
rates than that for single standing CNTs under a variety of flow conditions and in the size range from 76 to
500 nm. The lung deposition and the toxicity are both dependent on the CNT shape and form. Our study il-
lustrates the necessity to consider the CNT morphology and agglomeration status in the evaluation of the air-
borne CNT health impact. The comparison between the developed lung deposition model and previous empirical
study results showed that the particle deposition in the lung is mainly determined during inhalation.

1. Background
Filtration and inhalation models of aerosols, such as engineered
nanoparticles, medicines, bacteria and viruses, have been discussed
extensively in the last decades. Because both filtration and inhalation
modelings are significant for preventing of inhalation exposure to toxic
particles as asbestos fibers or viruses like SARS-CoV-2 (COVID-19), and
curing a respiratory disease through an inhalation therapy (Basile,
2020; Ma-Hock et al., 2013; Fathizadeh, 2020; Donaldson and Tran,
2004; Oberdörster et al., 2015). Carbon nanotubes (CNTs) are used to
reinforce and enhance the mechanical or electrical properties of ma-
terials (e.g. CNT-polymer or concrete composites). The global CNT
market is anticipated to double in 2020 compared to 2015, when the
annual market sale was $2.26 billion (Kim et al., 2017). Health con-
cerns for workplaces, laboratories exposure and emitted CNTs from
CNT-containing products also intensify with the CNT market growth. In
addition to such concerns regarding released CNTs, recent research
papers present CNTs or rod-shape carbon particles from internal com-
bustion processes, such as diesel engines, wood burning, natural gas
power plant and propane kitchen burner (Jung et al., 2013; Murr and
Garza, 2009; Swanson et al., 2016).
A number of studies showed the asbestos-type pathology associated
with exposure to long and straight CNTs (Muller et al., 2009; Poland
et al., 2008; Takagi et al., 2008). Davis et al. (1986) have studied the
effect of the geometrical length on pathogenicity of asbestos fibers and
showed high toxicity caused by long fibers through their experimental
investigation. Moreover, a number of studies found that inhaled CNTs
possessed cytotoxicity, inflammatory cell influx and potential to pro-
mote lung tumors (Ma-Hock et al., 2013; Shvedova et al., 2008; Li et al.,
2007; Porter et al., 2012; Sargent et al., 2014). Furthermore, Erdely
et al. (2009) showed that CNTs were able to cause immunosuppression
and inflammation, and change molecular signaling in extra pulmonary
tissues.
These toxicity research results also motivated developments of nu-
merical models of airborne CNT lung deposition and filtration. For in-
stance, Wang et al. (2011) presented three different approaches to
predict filtration efficiencies of airborne CNTs through a screen filter. In
their model, they assumed CNTs as fibrous particles with certain aspect

⁎
Corresponding author at: Institute of Environmental Engineering, ETH Zurich, 8093 Zurich, Switzerland.
E-mail address: yeonkyoung.bahk@gmail.com (Y.K. Bahk).

https://doi.org/10.1016/j.impact.2020.100240
Received 9 March 2020; Received in revised form 2 June 2020; Accepted 25 June 2020
Available online 11 July 2020
2452-0748/ © 2020 Elsevier B.V. All rights reserved.
T. Hammer, et al.
ratios and considered physical characteristics, such as orientations, the
effective interception length, aerodynamic diameter, etc. Sturm (2014)
followed the possible transport paths of CNTs to the alveoli and cal-
culated CNT depositions in the alveoli of the human respiratory tract
(HRT). In the study, the effects of different tube diameters and aspect
ratios of CNTs were intensively investigated.
At the same time, some recent studies and publications showed that
realistic airborne CNT emissions do not only consist of single standing
(straight and curly) CNTs, but also comparable amount of agglomerated
or bended/coiled CNTs in sphere-like shapes (Chen et al., 2012; Canu
et al., 2020; Thompson et al., 2015; Bahk et al., 2013; Wang et al.,
2015). Chen et al., 2012 reported that CNTs tend to agglomerate in
different shapes. The most frequent shapes were isometric CNT ag-
glomerates (sphere like particles), single standing CNTs and few irre-
gular shaped particles.
Similar to Chen et al., 2012 we separate fiber like CNT particles and
CNT agglomerates with sphere like shape. We addressed this fact of
more different shapes by considering single-standing-CNT-CNT ag-
glomerate mixtures. Our previous study showed that the higher con-
centration CNTs in a suspension, the higher fraction of aerosolized CNT
agglomerates in an air sample (Bahk et al., 2013). Characteristics of
airborne CNTs were also investigated through the fractal-like agglom-
erate models, which showed comparable results with measurement data
from electron microscopy (Wang et al., 2015). Buckley et al. (2012) also
reported the strong tendency of CNTs to form ‘broadly spherical’ par-
ticles when they were aerosolized.
In the present study, the existing filtration model and lung deposi-
tion model for fibrous particles were revised and advanced models for
both filtration and deposition for realistic airborne CNTs with ag-
glomerate characteristics were introduced. The filtration model was
applicable to airborne CNT mixtures with various single-to-agglomer-
ated-CNT ratios, and was validated experimentally. Then the same
approach, using the single-to-agglomerated-CNT ratios, was applied to
the lung deposition model for airborne CNTs.
2. Methods
In this study, we employed a fractal model for CNT agglomerates
(Wang et al., 2015) and took into consideration the CNT agglomerate
fraction in the airborne CNT mixture. The fractions were obtained by
SEM (scanning electron microscope) image analysis of sampled aero-
solized CNTs (Baytubes, Bayer Material Science, Germany) from a li-
quid suspension. We employed CNTs that had 15–20 nm diameters and
1–10 μm lengths. However, after the functionalization processes, which
improved CNT dispersion in water, the lengths were shortened to sev-
eral μm or sub-microns. The filtration model for the twilled dutch wire
mesh (Sachinidou et al., 2017) and the lung deposition models devel-
oped by Asgharian and Anjilvel et al. for spherical and fibrous particles
(Anjilvel and Ashgarian 1995; Asgharian et al., 1988) were revised, and
advanced models were developed in combination with the agglomer-
ate's characteristics. Fig. 1 shows the flow chart for the CNT filtration
and lung deposition models. Fig. 1 consists of two parts. The left part
shows a combination of all factors that were considered in order to
evaluate filtration of CNTs with all different shapes (single standing
CNT, CNT agglomerate, single standing CNT-CNT agglomerate mix-
ture). Hereby factors such as the CNT mixing states, the CNT fractal
model, feed into the filtration model and the outcome of the filtration
model is the CNT collection efficiency. The right part shows the lung
deposition of CNTs considering all different configurations (single
standing CNTs, CNT agglomerates and single standing CNT-CNT ag-
glomerate mixtures). Similar to the filtration part, CNT mixing states
and the fractal model were considered for the CNT exposure assess-
ment. In addition, different exposure scenarios (light or heavy
breathing) for the CNT deposition in the lung were considered in the
assessment of CNT exposure.
In order to verify the applied filtration model for CNTs
2
NanoImpact 19 (2020) 100240
experimentally, a basic filtration set-up was used as shown in Fig. 2.
Airborne CNT mixtures were generated by an aerosol generator (TSI
3079a). The water droplets were dried by a diffusion dryer. A differ-
ential mobility analyzer (DMA, TSI 3082) was used to classify the CNTs
according to their electrical mobility diameters and an ultrafine con-
densation particle counter (uCPC, TSI 3076) counted the CNT number
concentration for each mobility diameter upstream and downstream of
the filter holder. A steel twilled dutch wire mesh (solidity 0.62; average
wire size 0.31 μm) was used as the filter. The face velocity was 5 cm/s.
The filtration efficiency is calculated as the following:
Cup − Cdown
Ef _ exp = ,
Cup (1)
where Cup and Cdown are the upstream and downstream concentrations
of airborne CNT mixtures, respectively.
2.1. Agglomerate fraction in the airborne CNT mixture
In order to determine the agglomerate fraction in the airborne CNT
mixture, CNTs were aerosolized and collected on silicon substrates for
SEM analysis. The airborne CNTs were classified by the DMA to dif-
ferent electrical mobility diameters, such as 76, 90, 110, 150, 200, 300,
400 and 500 nm. Single standing CNTs are normally aligned to the air
flow, thus they were in the same size range when they had the same
electrical mobility diameters. Even if agglomerated CNTs have different
shapes and different geometrical sizes, the same electrical mobility size
can represent their physical properties for the deposition on the filter or
in the lung. The collected samples were analyzed by SEM and the
fraction of single standing CNTs for each mobility diameter was ob-
tained with the commercial image analyzing software (Image J). Fig. 3
shows some examples of the SEM images. The sample with larger mo-
bility diameter shows more collected CNT agglomerates. More than 300
images were taken by SEM and analyzed to reduce uncertainties. The
obtained data were fitted to an exponential line as shown in Fig. 4 to
determine the relationship between the mobility diameter and the
fraction of single standing CNTs in the classified mixture. As presented
in Fig. 4, the fraction of single standing CNTs (fS_CNT) decreased with
increasing mobility diameter of airborne CNTs. The obtained relation
(represented in formula 2) was applied to the deposition model and is
expressed as:
Single standing CNT fraction, fS _ CNT = 2.00 exp( −0.01dm), (2)
where dm is in nm. The applicable range started from 76 nm towards
bigger mobility diameters. Below 76 nm the fraction of single standing
CNTs was considered as 100%. We assumed that the form of the other
airborne CNTs in this mixture were CNT agglomerates, which were
considered as sphere-like particles based on Fig. 3.
3. Models
3.1. Filtration model
The single fiber filtration model was employed in the study. Based
on the twilled dutch wire mesh model (Sachinidou et al., 2017), dif-
ferent filtration mechanisms caused by diffusion (ED), interception (ER),
interception of diffusing particles (EDR) and impaction (EI) were con-
sidered in the model. The detailed equations for spherical particles are
shown in Eqs. (3) to (8).
2
ED = 2.7Pe− 3 , (3)
1.24R2/3
EDR = ,
(KuPe )1/2 (4)
1 − α R2
ER = ,
Ku 1 + R (5)
T. Hammer, et al. NanoImpact 19 (2020) 100240

Fig. 1. A flow chart to develop precise models for CNT filtration and lung deposition. The applied filtration model and the lung deposition model for airborne CNT
mixtures were based on the existing filtration and lung deposition models, the CNT agglomerate status, and the model for agglomerated CNTs. Exposure scenarios
were added to estimate CNT deposition.

Fig. 2. A schematic of the filtration set-up. The set-up contains atomizer, diffusion dryer, DMA (differential mobility analyzer), Kr-85 (neutralizer), 3-way valves
connected to a filter (holder) and uCPC (ultrafine condensation particle counter), needle valve to control the flow rate, HEPA (high efficiency particulate air) filter,
flowmeter and pump.

EI =
1
[(29.6 − 28a0.62) R2 − 27.5R2.8] Stk , R = dp/df, U0 is the face velocity on the filter surface, df is the fiber
(2Ku)2 (6) diameter, dp is the particle diameter, α is the solidity of the filter, t is
filter thickness and D is diffusion coefficient of particle. The filtration
Ef = ED + ER + EDR + EI , (7) model for single standing CNTs (Wang et al., 2011) was implemented
using the following parameters:
The total filtration efficiency is
3
−4α ∙ Ef ∙ t ρCNT dCNT Cc U0
Stk = , is the stokes number,
Ef total = 1 − e π ∙ df ∙ (1 − α ) , (8) 18μdf Ra (9)
df U0 3πμ
where Pe = D = df U0 kTC dp ,
is the Peclet number, where k is the and RCNT = LCNT sin 40° /df , is the effective radius of a CNT fiber,
c (10)
Boltzmann constant, T is the absolute temperature and μ is the viscosity
ρp dp2 Cc U0 dCNT β
of air, Stk = , is the stokes number, where Ra = Ra1sin2ψ + Ra2cos2ψ, Ra1 = 3[ln(2β ) − 0.5]
and
18μdf
2dCNT β
Ku = − 0.5 ln α − 0.75 − 0.25α + α, is the Kuwabara number, 2
R a2 = 3[ln(2β ) + 0.5]
.

3
T. Hammer, et al.
Fig. 3. SEM images of sampled airborne CNTs with 200 nm and 400 nm electrical mobility diameters (left and right, respectively). Airborne CNTs were classified by
the DMA and collected on a silicon substrate using a nanometer aerosol sampler (TSI 3089).
Ra1 and Ra2 are defined for a parallel and perpendicular fiber or-
ientation within the gas flow, respectively. The angle ψ for the random
orientation was taken as 54.74° (26). β is the aspect ratio and
ρCNT = 2.7001 ∙ dp−0.493 is the effective density of CNTs. dp is the se-
lected electrical mobility diameter in the DMA. Detailed calculations
may be referred to Wang et al. (2011).
The total filtration efficiency for airborne CNT mixtures calculated
by the applied filtration model is:
Ef _ CNT _ mixture = fS _ CNT Ef _ single _ standing _ CNT + (1 − fS _ CNT ) Ef _ sphere
(11)
where fS_CNT is the fraction of single standing CNT, and (1 − fS_CNT) is
the fraction of spherical agglomerates in the single-standing CNT-CNT
agglomerate mixture. fS_CNT decreases with increasing mobility dia-
meter dp, whereas (1 − fS_CNT) increases.
In the applied filtration model for airborne CNT mixtures, we as-
sumed that CNT agglomerates were sphere-like particles according to
the SEM images as shown in Fig. 3. Therefore, we used the sphere
model to calculate the filtration efficiency for the agglomerate CNTs.
Fig. 4. Fraction of single standing CNTs in airborne mixture as a function of the classified electrical mobility diameter. The fraction was obtained by an image
analyzing software (ImageJ) and the data were well fitted by an exponential line.
4
NanoImpact 19 (2020) 100240
3.2. Lung deposition models
The lung structures used in previous studies (Raabe et al., 1976; Yeh
and Schum, 1980) were all based on the morphometric measurement by
Raabe et al. (1976) and Yeh and Schum (1980) presenting results for
simplified geometries of the entire lung. The morphological parameters,
such as length, diameter, branching angle, number of airway tubes and
gravity angle from Yeh and Schum's study (1980) were employed in this
study. The used data are presented in Table 1. It includes information
for every generation from respiratory bronchioles, alveolar ducts to
alveoli. As described in Table 1, the human lung has been commonly
described as two main assembled parts, i.e. the conducting zone and
transitional and respiratory zones. These zones are also termed tra-
cheobronchial (TB) and alveolar (AL) region, respectively. The TB re-
gion includes generations from 1 to 16 and AL region includes gen-
erations from 17 to 23 (Weibel, 1966).
The lung deposition model contains depositions in head (nasal),
tracheobronchial and alveolar regions. The particle depositions in the
airways are caused by diffusion, sedimentation, impaction and inter-
ception. For single standing CNT deposition, the theory for the fiber
deposition was taken into account in the present model.
T. Hammer, et al. NanoImpact 19 (2020) 100240

Table 1 1 2β2 − 1
β3 ⎡ ln(β + β 2 − 1 ) − β⎤ c 1
Typical path lung model for human and description of bronchiole and alveolar 3 ⎢
⎣ β2 − 1 ⎥
⎦ ,
generations (Yeh and Schum, 1980; Weibel, 1966). L is an airway segment b1 =
4 β2 − 1 (16)
length, d is a segment diameter, θ is a bifurcation angle and ϕ is a gravitational
angle.
1 2β2 − 1
Tracheobronchial Generation (n) Number of L (cm) dair (cm) θ ϕ
β3 ⎡ ln(β + β 2 − 1 ) + β⎤ c2
3 ⎢ ⎣ β2 − 1 ⎥
⎦ ,
region tubes b2 =
8 β2 − 1 (17)
bronchi ↑ 1 1 10 2.01 0 0
2 2 4.36 1.56 33 20 where β is the aspect ratio of CNTs. The correction factors c1 and c2
3 4 1.78 1.13 34 31 were derived by Asgharian and Yu (1989) as 1.142 and 0.558, re-
bronchioles 4 8 0.965 0.827 22 43 spectively.
terminal bronchioles 5 16 0.995 0.651 20 39
Even if the particle mobility size is small, fibrous particles with a
6 32 1.01 0.574 18 39
7 64 0.890 0.435 19 40
high aspect ratio like CNTs, can be deposited by interception.
8 128 0.962 0.373 22 36 Therefore, the deposition efficiency, due to combined mechanisms of
9 256 0.867 0.322 28 39 impaction and interception, was used in the model for CNTs and Nimp
10 512 0.667 0.257 22 45
+int, which was derived by Ding et al. (1997) as:
11 1024 0.556 0.198 33 43
12 2048 0.446 0.156 34 45 b
(χ + 3.5LCNT )a ⎤
13 4096 0.359 0.118 37 45 Nimp + int = ⎡ ,
14 8192 0.275 0.092 39 60 ⎢
⎣ c + (χ + 3.5LCNT ) ⎥
a
⎦ (18)
15 16,384 0.212 0.073 39 60
↓ 16 32,768 0.168 0.060 51 60 where LCNT is the length of CNTs and represented by the outer diameter
Alveolar region ↑ 17 65,536 0.134 0.054 45 60 of CNT agglomerates following a model from (Wang et al., 2015).
respiratory 18 131,072 0.120 0.050 45 60 For very small particles, e.g. particle mobility size below 100 nm,
bronchioles
19 262,144 0.092 0.047 45 60
the diffusion effect is dominant for deposition (Hinds 1998). Cheng
alveolar ducts 20 524,288 0.080 0.045 45 60 et al. (1993) proposed the expression for the particle deposition due to
21 1,048,576 0.070 0.044 45 60 diffusion as:
22 2,097,152 0.063 0.044 45 60
1
alveolar sacs ↓ 23 4,194,304 0.057 0.043 45 60
(
Ndif = 1 − exp −CD 2 Q− 8 ,
1
) (19)

where C is a constant and was obtained by Cheng et al. (1993) as 12.65

Due to the complex structure and lack of knowledge on the anato-
for human. D is the particle diffusion coefficient of the diffusing particle
mical structure and flow field in the nasal region, prediction of de-
(spheres, fibers, etc.). For CNTs it can be expressed as:
position in the nasal region was obtained empirically. Zhang and Yu
(1993) established the particle deposition efficiency for spherical par- kT 1 2
D= ⎛ b1 + b2⎞,
ticles in nasal region based on experimental data from Raabe et al. 3πμd v ⎝ 3 3 ⎠ (20)
(1977) and Raabe et al. (1988). The deposition efficiency Nimp due to
impaction is expressed as: where k is the Boltzmann constant, T is the absolute temperature, μ is
the viscosity of air and dv = 0.7795 ∙ dp0.9692 is the fiber volume
b equivalent diameter.
(da2 Q)a ⎤
Nimp = ⎡ , The total efficiency Nnasal in the nasal region is expressed as follows:
⎢ c + (da2 Q)a ⎥ (12)
⎣ ⎦
for spherical particles,
where a, b and c are constants and da is the aerodynamic diameter of Nnasal = 1 − (1 − Nimp )(1 − Ndif ), (21)
particles in μm and Q is the air flow rate in cm3/s. a and b for human are
1.257 and 0.609, respectively, c is 10,000 for all animals. Q was ob- for CNTs,
tained from the average weight of human, 70 kg, using the Guyton
Nnasal = 1 − (1 − Nimp + int )(1 − Ndif ). (22)
formula (Zhang et al. 1993;32, Guyton, 1947):

3
Q = 0.15 W 4 ,
where W is the weight of mammal in grams.
For fiber deposition in the nose, the effect of fiber shape on the
particle Stokes number was considered and applied to Eq. (12). The
constants a, b and c are the same as in Eq. (12).
For the lung airways, deposition due to sedimentation is considered
(13) additionally. The deposition model shares equations for tracheobron-
chial and alveolar region with different input parameters. The deposi-
tion efficiency due to diffusion was derived for spherical particles by
Ingham (1975) as:
ηd

b
= 1 − 0.819 exp( −14.63∆) − 0.097 exp( −89.22∆) − 0.0325
(χ )a ⎤
Nimp = ⎡ , exp( −228∆) − 0.059 exp −125.9∆3 , ( 2
)
⎢
⎣ c + (χ )a ⎥
⎦ (14) (23)

where,
where,
DL
1 ∆= ,
χ= (b1 + 2b2 ) ρCNT d v2 Q, 4UR2 (24)
3 (15)
where L and R are the airway length and radius, respectively, U is the
where dv = 0.7795 ∙ dp0.9692 is the fiber volume equivalent diameter, Q average flow velocity in the airway. D is the diffusion coefficient. For
is the air flow rate in cm3/s, ρCNT is the CNT density, b1 and b2 are the deposition of CNTs, we use the diffusion coefficient of CNTs D, which is
normalized fiber mobilities for parallel and perpendicular movement to described in formula 20.
the flow direction (representing random fiber orientation), expressed The deposition efficiency in the airways due to sedimentation ac-
as: cording to Pich's expression (Pich, 1972) was derived as:

5
T. Hammer, et al. NanoImpact 19 (2020) 100240

2
ηs =
π ( 1 1 2 1
2ε 1 − ε 3 − ε 3 1 − ε 3 + sin−1 ε 3 , ) (25)
containing mostly single standing CNTs or predominantly CNT ag-
glomerates.
where, The particle depositions in the different regions along the lung
airways were investigated separately and linked afterwards. For ex-
3 L Vs ample, when particle deposition in the TB region was considered, the
ε= ,
8 RU (26) nasal deposited amount was excluded as in the following equation (Eq.
where Vs is the terminal settling velocity of CNTs and expressed as: (34)).

ρ0 da2, CNT gCc ηtotal _ TB _ final = (1 − ηtotalnasal )ηtotal _ TB . (34)

Vs = ,
18μ (27)
The final particle deposition in the alveolar regions was expressed
where ρ0 is a standard particle density (1 g/cm3), da,CNT is the aero- as:
dynamic diameter for CNT, g is the gravitational acceleration and Cc is
ηtotal _ alveolar _ final = (1 − ηtotalnasal )(1 − ηtotal _ TB )ηtotal _ alveolor . (35)
the Cunningham slip correction.
Cai and Yu (1988) derived the deposition efficiency for impaction of We have specifically considered particle deposition during inhala-
single standing CNT fibers by: tion in order to compare the new advanced model that considers single
8 sin αb f1 standing CNT- agglomerated CNT mixtures to the conventional single
ηi = Stk , fiber CNT models. However, the full exposure model including de-
Rd / Rp f0 (28)
position during pause and exhalation process needs to be studied in the
where Rd and Rp are the radii of the daughter tube and parent tube, future.
respectively. The parent tubes are the upper generation tubes in the
lung model, from which the lower generation tubes (daughter tubes) 3.3. Validation of lung deposition model
originate and double in number.
2 In order to validate our data from deposition model, we compare the
π 5 8 R
f0 = π − ⎛ + ⎛ π − ⎞ cos2 αb ⎞ ⎜⎛ d ⎟⎞ , data from our calculation results for spherical particles with emperical
⎝ 4 ⎝ 4 3 ⎠ ⎠ ⎝ Rp ⎠ (29) data from Heyder et al. (1986). We compared deposited particle frac-
tions in the different regions of the respiratory tract in the respective
f1
size range of 75 nm to 475 nm under the sitting breathing scenario. Our
2
1 11 sin αb ⎞ ⎛ Rd ⎞ ⎛ modeled data for deposition of spherical particles fits well to experi-
= 1 + ⎛− + ⎛π − ⎞ cos2 αb − ⎜ ⎟ + ⎜

⎝ 3 ⎝ 3 ⎠ 3 ⎠ ⎝ Rp ⎠ ⎝ mental values for alveolar deposition from Heyder et al. (1986). In the
2 π sin 2α 15 7 π alveolar region, calculated and experimental depositions start at a value
⎛ − ⎞ cos2 αb + b
+ ⎛6 − π ⎞ cos4 αb + ⎛ − ⎞ sin2 αb of 40% at a diameter of 75 nm and show a similar decreasing trend
⎝3 8⎠ 5 ⎝ 8 ⎠ ⎝ 15 8⎠
2 towards bigger diameters (Fig. 7). At 475 nm spherical particles with
R
cos2 αb ⎞ ⎜⎛ d ⎟⎞ ,
⎟
unit density from Heyder et al. (1986) deposit for 12% and our calcu-
⎠ ⎝ Rp ⎠ (30) lated depositions for spherical particles show values of around 8%.
Thus, calculated and experimental depositions are very close. In addi-
and αb is the bifurcation angle and Stk is the particle Stokes number
tion, the total deposition curves of simulated (Fig. 8) and experimental
which is given by Anjilvel and Asgharian (1995) as:
data show similar shapes. Starting at about 45%, decreasing towards
1.142ρd v2 βU bigger diameters, and reaching an almost constant level at about
Stk = .
36μR 0 (31) 275 nm. Thus, simulated deposition could be validated by experimental
data.
The total efficiency ηtotal for spherical particles (agglomerates) or
fibers can be expressed as:
4. Results
ηtotal = 1 − (1 − ηd )(1 − ηs )(1 − ηi ) (32)
In the calculations for CNTs, physical parameters may be referred to 4.1. Advanced filtration model
our previous study (Wang et al., 2015).
Similar to Eq. (11), total deposition for CNT mixtures can be cal- Filtration efficiencies by the wire mesh for spherical particles, single
culated as: standing CNTs and CNT mixtures (including CNT agglomerates and
single standing CNTs), which is a more realistic model for airborne
ηtotal _ CNT _ mixture CNTs, were calculated. The filtration efficiency of the wire mesh against
= fS _ CNT ηtotal _ single _ standing _ CNT + (1 − fS _ CNT )ηtotal _ CNT _ agglomerate CNT mixtures was experimentally obtained. Obtained filtration effi-
ciencies in the size range of 50 nm to 500 nm were compared and
(33) shown in Fig. 5. Compared with the sphere model, CNT filtration effi-
Particle depositions in the airways of the human lung were calcu- ciencies showed higher collection efficiency in the entire range. The
lated for airborne particles with different morphologies such as sphe- experimental filtration results of the CNT mixtures (mixtures of single
rical particles with unit density (1 g/cm3), CNT agglomerates, single standing CNTs and CNT agglomerations, with size dependent ratio of
standing CNTs and CNT mixtures of agglomerated and single standing single standing CNT and CNT agglomeration) showed almost the same
CNTs. Three different breathing scenarios such as sitting breathing, filtration efficiencies compared to the modeled filtration efficiencies for
light working (doubled amount of the flow rate as the sitting breathing single standing CNTs for sizes of about 50 nm. With increasing mobility
condition) and heavy working conditions (tripled amount of the flow diameters, the differences were getting bigger. Then the differences
rate as the sitting breathing condition) were applied. The airflow rates between the sphere model and the empirical data stabilized and even
for each condition were 646, 1291 and 1937 ml/s, respectively. The slightly decreased. As shown in Fig. 5, single standing CNT model
particle mobility diameter range from 76 nm to 500 nm was chosen for showed a reasonable agreement for the particle sizes smaller than
estimating the particle deposition, because the typical size distribution 100 nm, but for the larger sizes, it overestimated the collection effi-
of the used airborne CNTs, generated in the experiments of the present ciencies compared with the experimental results. The developed ad-
study, showed the same size range and the size range included mixtures vanced model that considers single standing CNT-CNT agglomerate

6
T. Hammer, et al.
Fig. 5. Comparison of CNT filtration efficiencies. Filtration efficiencies for each
model and experimental result are shown as functions of the electrical mobility
diameter. Curves are calculation results of the models for spherical particles,
single standing CNTs, airborne CNT mixtures single standing CNTs and CNT
agglomerates (named advanced CNT model) and the results of CNT filtration
experiments are represented by dots.
mixtures showed a good agreement with the empirical results except for
the size range around 50 nm, for which there was a small over-
estimation. For increasing particle mobility diameters, the estimation
for the filtration efficiency by the advanced model was similar to that of
the sphere model, just slightly larger.
4.2. Advanced lung deposition model
In the advanced lung deposition model, we assume that realistic
airborne CNT particles are mixtures of single standing CNTs and CNT
agglomerates. The fraction of CNT agglomerates increases with in-
creasing mobility diameter that was selected at the DMA. Particle de-
positions in the conducting zone were estimated through the models
mentioned in the methods part. The results are shown in Fig. 6. De-
positions of spherical particles and CNT agglomerates showed close
values in the particle size range below 100 nm, however, discrepancies
between them were getting bigger with increasing particle mobility
diameter. Nasal depositions increased with the particle size in the in-
vestigated size range for all models, but the increasing rates varied. The
highest particle deposition (37%) in the conducting zone occurred at
500 nm particle of spherical model in the nasal region under the heavy
working condition and the lowest one (0.04%) appeared for around
76 nm mobility size single standing CNT model under the sitting
breathing condition also in the nasal region. In the TB region, the model
of CNT mixtures showed a weaker decreasing trend with an increase of
particle mobility diameter than all other models in the entire in-
vestigated size range of 76 nm to 500 nm. The deposition lines of CNT
mixtures, as a function of mobility diameters in the TB region, were
almost flat in the size range.
The sitting breathing condition showed around two times higher
depositions than those under the heavy working condition (Fig. 7). For
example, for 76 nm spherical particles under sitting breathing and
heavy working conditions, the results showed 39.1% and 20.4% of
deposition fractions, respectively. Under the heavy working condition,
the deposition was much lower.
The particle deposition decreased with the particle size for all cases.
The particle depositions of spheres and CNT agglomerates showed al-
most the same values in the whole size range, which were also close to
CNT mixture depositions for the large particle sizes. Depositions of the
single standing CNTs were less than half of the values for spherical
7
NanoImpact 19 (2020) 100240
particles under all three breathing conditions. In general, CNT lung
deposition models showed lower deposition fractions than spherical
particles mainly due to diffusion deposition compared to spherical
particles.
Bigger CNTs have lower diffusion coefficients (as calculated in Eq.
(20)) than the spheres with the same mobility particle sizes, because
fibrous particles like CNTs have different diffusion coefficients de-
pending on their orientation distributions (Wang et al., 2011; Asgharian
et al., 1988). The diffusion deposition was significant in a small particle
size range and sedimentation and impaction depositions were sig-
nificant in a large particle size range.
These mechanisms led to deposition fraction differences between
spherical particle model and CNT models in the conducting zone
(Asgharian and Yu, 1988; Hinds, 1998).
Lung deposition can be compared via different metrics e.g. lung
deposited particle fraction (number based), the lung deposited surface
area (LDSA) or by mass in concentration or amount. LDSA or mass
would allow a toxicity assessment. Since the lung deposited particle
fraction corresponds to the filtration efficiency in filtration experi-
ments, we focused our investigation on the evaluation of the deposited
particle fraction in the lung.
Total particle collections in human lung airways were calculated
with above regional deposition data. Fig. 8 presents the results.
The total deposited fraction in the whole airway, which was cal-
culated for each particle size, decreased with increasing breathing air-
flow rate. The highest deposition value (45.5%) was for spherical par-
ticles at the smallest particle size under the sitting condition and the
lowest deposition (5.5%) was for single standing CNTs at the largest
particle size under the light working condition. Under the heavy
working condition, the highest deposited fraction for the CNT mixture
model was 29.5% at 500 nm, and the particle size range with the lowest
deposition for CNT mixtures was from 76 nm to 270 nm. Although the
deposited fraction was lower, the deposited amount would be higher
considering the following parameters such as duration of exposure
airflow rate. For the same duration of exposure, different breathing
scenarios lead to various total inhaled air amounts, and affect the de-
posited particle amounts. For heavy working and light working condi-
tions the tripled and doubled breathing airflow rates compared to the
sitting condition were considered, which would affect the deposited
amount.
In order to understand potential harmful effects of the airborne
CNTs better, above results were summarized in two different zones,
which are the conducting zone combining the nasal and TB regions and
respiratory zone (alveolar region). A reason to divide the two zones is
that the particle deposition in the alveolar region causes critical health
issues, while deposited insoluble particles in the conducting zones are
cleared out by sneezing or the mucociliary clearance process of the TB
region (Lippmann and Schlesinger, 1988; NIOSH, 2011). Comparable
with deposition fractions in the conducting zone (nasal and TB), al-
veolar depositions showed similar trends: higher deposition for smaller
particles. In the conducting zone, CNT mixtures model showed in-
creasing trends under all conditions, while spheres and CNT agglom-
erates showed deceasing trend from 76 nm to 150 nm (Fig. 9 a) and
increasing trend from 150 nm to 500 nm. Single standing CNTs showed
almost no changes on the deposited fraction. Under the sitting
breathing condition for the conducting zones, particle depositions were
relatively flatter than other breathing conditions in the entire size
range. The other two conditions showed deposition increases with in-
creasing particle size. Alveolar deposition for small size particles were
much higher than in the conducting zone, but for large size particles,
they showed much lower deposition values compared to the conducting
zone.
Finally, the model results for CNT deposition including CNT mixing
states were summarized in Fig. 10. Only CNT mixture model results
were selected from the results presented in Fig. 9. Increasing breathing
airflow rate lead to decreasing the depositions in the alveolar region.
T. Hammer, et al. NanoImpact 19 (2020) 100240

Fig. 6. Particle depositions in the nasal and tracheobronchial regions under different breathing scenarios. Particle depositions in the nasal and tracheobronchial
regions were calculated for spherical particles, CNT agglomerates, single standing CNTs and CNT mixtures (mixtures of single standing CNTs and CNT agglomerates)
under the sitting breathing condition (646 ml/s), light (1291 ml/s) and heavy working (1937 ml/s). The particle mobility diameter range from 76 nm to 500 nm was
used.

However, in the conducting zone the particle depositions increased
with increasing breathing airflow rate. In the alveolar region, smaller
particles led to higher depositions than larger particles, while opposite
trends were observed in conducting zone; thus, bigger particles were
deposited more easily in the conducting zone and small particles were
deposited more easily in the alveoli. The highest (26.8%) and lowest
(2.4%) deposition fractions were at particle sizes 500 nm and 76 nm
under the heavy working condition, respectively.
5. Discussions
The purpose of this study was the evaluation of particle collection
on filters and in the human lung not only for CNTs, but also for fibrous
particles, which have strong tendency to bend, coil or agglomerate.
Chen et al., 2012 found that CNTs tend to agglomerate in different
shapes (mainly sphere like CNT agglomerates and some irregular
shaped aggregates). Based on Chen et al., 2012 who recommended a
separation of single standing CNT and isometric particles (sphere like
particles) we applied mixing states of agglomerated and single standing
CNTs in air in the revised filtration and lung deposition models.
Besides the purpose to develop precise filtration model for airborne
CNTs, another important reason for this study was to show that it is
important to consider the CNT agglomerate ratio using single standing
CNT-CNT agglomerate mixing states that resembles realistic aerosols. It
could be simulated using traditional numerical models and validated by
application in the filtration model. Because filtration experiments could
be performed more easily than lung deposition tests, we compared
calculated results and empirical results to evaluate the model and va-
lidated the approach at a realistic level. Nevertheless, our quantitative
analysis of the CNT mixing states is primarily applicable to our study,
but the general approach can also be applied for other studies, where
the relationship between single standing and agglomerated CNT ag-
glomerates needs to be determined for each specific case.
The applied filtration model showed good agreement with experi-
mental results, while single standing CNT model showed large dis-
crepancies with experimental results as shown in Fig. 5. This big dif-
ference was caused by several reasons. The most critical point was the
mixing state of agglomerates and single standing CNTs. As presented in
Fig. 4, the fraction of agglomerated CNTs increases with an increase of
mobility size of the CNTs. For smaller particle sizes below 75 nm, dif-
fusion collection was the dominant mechanism, so the same mobility
size particles showed similar collection efficiencies (35). The single

8
T. Hammer, et al. NanoImpact 19 (2020) 100240

Fig. 7. Particle depositions in the alveolar region under different breathing scenarios. Particle depositions in alveolar region in the human lung were calculated for
the spherical particles, CNT agglomerates, single standing CNTs and CNT mixtures under the sitting breathing condition (646 ml/s), light (1291 ml/s) and heavy
working (1937 ml/s).

standing CNT model overestimated the filtration of CNTs especially for Although the applied model for CNT mixtures showed reasonably good
large particles, because curled or bended CNTs or CNT agglomerates agreement in the entire range, there was small underestimation of CNT
were not taken into account (Wang et al., 2011). With these structural penetration in the size range below 100 nm. Due to high fraction of
changes, the CNTs behaved similarly to compact spheres-like particles. single standing CNTs in small mobility size range this might be caused

Fig. 8. Total particle depositions in the airway into the human lung under different breathing scenarios. Total particle depositions in the human lung were calculated
for the spherical particles, CNT agglomerates, single standing CNTs and CNT mixtures under sitting breathing condition (646 ml/s), light (1291 ml/s) and heavy
working (1937 ml/s) conditions.

9
T. Hammer, et al. NanoImpact 19 (2020) 100240

Fig. 9. Regional total deposition in airway into the human lung. Total particle depositions in the conducting zone (including nasal and TB region) and alveolar region
were estimated through the model. Deposition fractions of spherical particles, CNT agglomerates, single standing CNTs, and CNT mixtures under different breathing
scenarios were compared with different mobility diameters, such as 76, 150, 300 and 500 nm.

by alignment effects of single standing CNTs along the airflow direc-

Fig. 10. Summary of CNT mixture deposition in airway into the human lung
under different breathing scenarios. Depositions of CNT mixtures in the con-
ducting zone and alveolar region under different breathing scenarios were
calculated as a function of electrical mobility diameters of airborne CNTs and
compared in each selected size, 76, 150, 300 and 500 nm.
tion, which could reduce the collection efficiency. Since the drag
coefficient of single standing CNTs is dependent on their orientation,
also the filtration efficiency was affected. This has not been considered
in the filtration models. Another potential reason is that the sample air
contained residues from water used to prepare CNT suspension and
usual size distribution of residues in water was overlap with airborne
CNT size distribution (Bahk et al., 2013). Using the collected SEM
images we identified a small fraction of particles in the small particle
range as residues, which were more sphere-like particles, and led to the
underestimation of CNT filtration efficiency (Chen et al., 2014; Wang
et al., 2015).
The revised lung deposition model which only models inhalation fits
well to Heyder’s (Heyder et al., 1986) experimental values, which re-
present deposition both during inhalation and exhalation, means that
the particle deposition in the lungs is mainly determined during in-
halation. In general, CNT lung deposition models with CNT mixtures
showed equal or in most cases lower deposition fractions than for
spherical particles, mainly due to less deposition by diffusion and se-
dimentation than for spherical particles. This comes from the fact, that
CNT particles have lower diffusion coefficients, for particles with small

10
T. Hammer, et al.
mobility diameters, compared to spherical particles with the same
particle mobility size, because fibrous particles like CNTs have different
diffusion coefficients depending on their orientation distributions
(Wang et al., 2011; Asgharian et al., 1988).
The diffusion deposition was significant in a small particle size
range and sedimentation and impaction depositions were significant in
the large particle size range. These mechanisms led to differences of the
deposition fraction of the spherical particle model and the CNT models
in the conducting zone (Asgharian and Yu, 1988, Hinds 1998). How-
ever, in the alveolar region, diffusion was the dominant deposition
mechanism in the entire size range and sedimentation contributed to
the deposition of particles in the large size end of the tested range of
76 nm to 500 nm. This is mainly due to slower flow velocity and longer
residence time for diffusion in airway of higher generation numbers
(Asgharian and Yu, 1988).
CNT depositions in the nasal increased with the increasing flow rate,
for example, the heavy working scenario showed the highest deposi-
tions. In contrast, the sitting breathing showed the highest CNT de-
positions in the rest of the conducting zone (TB) and alveolar region.
Based on Brody et al., 1981, fibrous particles are believed to mainly
deposit at the bronchioalveolar duct junction (BADJ). As aforemen-
tioned, CNT agglomerates are assumed as spherical fiber agglomerates
and thus behave differently as fibrous particles at the BADJ. The main
deposition mechanism for single standing CNTs at the BADJ is by in-
terception, which does not play role for spherical particles. Spherical
particles would simply slip into and be deposited in the alveoli. Com-
paring alveolar deposition values of spherical particles (spherical CNT
agglomerates) and single standing CNTs explains also why deposition
for spherical particles in the alveoli is much higher as that of single
standing particles.
6. Conclusions
We revised previous models and developed the models for realistic
CNT mixtures in air with a new approach using the mixing states of CNT
agglomerates and single standing CNTs. The SEM results showed that
the relative percentage of CNT agglomerates compared to single
standing CNTs increased with increasing particle diameter.
The developed filtration model and the approach were verified
empirically in the study. The calculated lung deposition for the realistic
CNT mixtures showed much higher deposition fractions than for single
standing CNTs under the different flow conditions and in the entire size
range.
The lung deposition and the toxicity are both dependent on the CNT
shape and form. The coiled CNT agglomerates might deposit more, but
their toxicity might be lower. Therefore, our study illustrates the ne-
cessity to consider the CNT morphology and agglomeration status in the
evaluation of the airborne CNT health impact.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgement
This study was partially supported by the Center for Filtration
Research (CFR) at the University of Minnesota (MN, US). The authors
thank Prof. Jing Wang for the fruitful discussion.
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