Advanced Powder Technology 25 (2014) 17481753

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Advanced Powder Technology

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

Original Research Paper

Particle size measurement of reference particle candidates and

uncertainty region of count and mass based cumulative distribution
Hideto Yoshida a,, Tetsuya Yamamoto a, Yasushige Mori b, Hiroaki Masuda c, Kenji Okazaki a,
Hirosuke Sugasawa d
a

Department of Chemical Engineering, Hiroshima University, 1-4-1, Kagamiyama, Higashi-Hiroshima, Hiroshima 739-8527, Japan
Department of Chemical Engineering and Materials Science, Doshisha University, 1-3 Tatara Miyakodani, Kyotanabe, Kyoto 630-0321, Japan
Kyoto University, Invited Special Research Fellow, Cooperative Research Center of Life Sciences, Kobe Gakuin University, Minatojima, Chuou-ku, Kobe 650-8586, Japan
d
Horiba, Co., Ltd., 2 Miyanohonmachi, Kisshoin, Minami-ku, Kyoto 601-8510, Japan
b
c

a r t i c l e

i n f o

Article history:
Received 10 March 2014
Received in revised form 28 June 2014
Accepted 1 July 2014
Available online 25 July 2014
Keywords:
Particle size
Reference particle
Uncertainty region
Log-normal distribution
Size measurement

a b s t r a c t
In order to conrm reliable particle size measurement technique and to prepare standard reference particles for calibrating particle size measurement devices, uncertainty region of count and mass based size
distribution have been theoretically examined. The uncertainty region of count base cumulative size distribution is smaller than that of the mass base cumulative distribution.
The uncertainty region of count base cumulative size distribution is nearly constant over wide range of
particle diameter and the region is nearly constant for sample size greater than about 20,000.
On the other hand, the uncertainty region of mass base cumulative distribution increases with the
increase of particle diameter.
The reliability of theoretical uncertainty region is conrmed by the experimental data of particle size
measurement.
2014 The Society of Powder Technology Japan. Published by Elsevier B.V. and The Society of Powder
Technology Japan. All rights reserved.

1. Introduction
Particle size distribution is measured by various methods such
as microscopy method, laser diffraction and scattering method,
dynamic light scattering method, electrical sensing zone method
and liquid sedimentation method. Though the laser diffraction
and scattering method, dynamic light scattering method and electrical sensing zone method have the advantage of shorter measurement time and good repeatability, but they need complicated
calibration by direct method [1,2]. In order to calibrate particle size
measurement devices, it is necessary to prepare standard reference
particles. For the reference particles, mono-disperse and poly-disperse particles are proposed. For the poly-disperse reference particles, Yoshida et al. measured particle size distribution of three
kinds of spherical glass beads by use of improved type sedimentation balance and microscopic methods with sample size less than
about 20,000 particles [3,4]. Mori et al. reported the results of
the round robin test for the two kinds of particles (MBP110, 10
100) [5]. This paper newly discusses the uncertainty region for

Corresponding author. Tel.: +81 82 424 7853; fax: +81 82 424 5494.
E-mail address: r736619@hiroshima-u.ac.jp (H. Yoshida).

count and mass based particle size distribution due to limited particle count number, measurement scale error and uncertainty of
nite dot size in a screen.
In order to represent particle size distribution measured by
microscopic method, uncertainty region must be estimated. On
this purpose, Masuda et al. derived analytical equation of the necessary sample size with any uncertainty region at mass median
diameter [6,7]. However, in order to know better information of
particle size distribution by microscopic method, it is necessary
to estimate uncertainty region over all the range of particle
diameter.
In this report, three kinds of particle size measurement of micro
beads barium titanate glass particles (MBP110, 330, 10100)
was conducted. The melted high temperature liquid solution of
lod shape was subjected into waterair jet and particles about
1 mm size were dried. Then particles were grinded and classied.
For the MBP110 particles, particles greater than 10 lm were classied by air-cyclone and sieve. For the MBP10100 particles, the
particles were grinded by vibrating mill and then classied by
sieve. Particle shape for the three kinds of particles is almost spherical shape and the aspect ratio is greater than about 0.99.
The previous report discusses particle size distribution with
sample size less than about 20,000 [3,4]. In order to increase the

http://dx.doi.org/10.1016/j.apt.2014.07.001
0921-8831/ 2014 The Society of Powder Technology Japan. Published by Elsevier B.V. and The Society of Powder Technology Japan. All rights reserved.

H. Yoshida et al. / Advanced Powder Technology 25 (2014) 17481753

1749

Nomenclature
m, b
n
q(b)(x)
q0, q3

parameter used in Eq. (3)

sample size ()
size frequency distribution of parameter b (/lm)
size frequency distribution based on count and mass,
respectively (/lm)
Q0, Q3
cumulative distribution based on count and mass,
respectively ()
u
reliability parameter ()
x
particle diameter (lm)
x50,0, x50,0 count median diameter and true count median diameter, respectively (lm)
x50,3, x50,3 mass median diameter and true mass median diameter, respectively (lm)

reliability of particle size distribution, sample size greater than

about 20,000 is necessary. This report presents the measurement
results with sample size about 50,000. The uncertainty region for
count and mass based size distribution is newly shown in the data.
Theoretical equation of uncertainty region over all particle diameter range is proposed and the reliability of uncertainty region is
newly conrmed by use of experimental data.

x m; b mean particle diameter dened by Eq. (3) (lm)

dx(0), dx(3) uncertainty of particle diameter based on count and
mass based cumulative distribution (lm)
a
parameter used in Eq. (4) ()
r, rg
standard deviation of log-normal distribution and geometric standard deviation, respectively ()
dQ0, dQ3 uncertainty region of count and mass cumulative distribution dut to limited sample size (-)
d0, d3
total uncertainty region of count and mass based
cumulative distribution (lm)
dp, dd
uncertainty due to measuring scale error and dot size
on screen, respectively (lm)

particle is divided into its original particles and size measurement

was carried out only for the original particles. For the measurement, the limitation of focus depth is considered as a dot size. Then
reliability of this measurement is considered to be high level.
3. Uncertainty region based on limited sample size
3.1. Uncertainty region of count base cumulative distribution

2. Microscopic method
Measurement of particle size distribution was carried out for
MBP110, 330 and 10100 particles. The size range of these particles are ranged from 1 to 10, 3 to 30 and 10 to 100 lm, respectively. Size measurement of the MBP particles was carried out by
scanning microscope (JSM-5600, Hitachi, Co., Ltd.).
In order to measure the length of particle size accurately, a certied scale shown in Fig. 1 (MRS-4.1, Geller Microanalytical Laboratory, Boston) was used for the measurement. The measuring
conditions of the three kinds of particles are as follows:

MBP1  10 mag: X1500 Sample size n 55728

MBP3  30 mag: X500 Sample size n 50685
MBP10  100 mag: X200 Sample size n 51002
Fig. 2 shows photographs taken by SEM and the size of each particle in these photographs was measured manually by marking a
suitable sized circle on the particle. In order to eliminate counting
error near the frames, size measurement was carried out only to
the particles having the center positions inside the screen. For
the overlapping particles on the counting process, the overlapped

In the case that total number of particles counted is equal to n,

the uncertainty of count base cumulative size distribution is calculated by the following equation [8].

r
Q 0 x 1  Q 0 x
d Q0 u
n

By use of Tschebyscheff theory which can be applied to general

frequency distribution, the parameter u is set to be 4.47 for 95%
reliability level. The uncertainty of particle size is calculated as
follows.

d x0

d Q 0 x
q0 x

where q0(x) is the density distribution by count.

3.2. Uncertainty region of mass base cumulative distribution
In order to obtain accurate particle size distribution, it is necessary to indicate uncertainty region over all particle size range.
Assuming particle size distribution follows a log-normal distribution, the following equation is obtained to the mean particle
diameter [6].

x m; b

Z
0

m1


m r2
xm qb x dx x50;b exp
2

In the above equation, r which equals to ln rg, indicates standard deviation of log-normal distribution.
For the size frequency distribution of q(b)(x), the parameter b
equal to 0 and 3 means count or volume based distributions,
respectively.
Let b equal to 0 in Eq. (3), the following equation is obtained.

x m; 0 x50;0 exp

a exp
Fig. 1. Certied scale for SEM measurement.



m

m r2
x50;3 exp
 3 r2 a x50;3
2
2

m

 3 r2
2

The uncertainty region for a particle diameter at a times of mass

median diameter is calculated by the following equation [9].

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H. Yoshida et al. / Advanced Powder Technology 25 (2014) 17481753

Fig. 2. Photographs of MBP particles (SEM).

1  d1 a x50;3 6 a x50;3 6 1 d1 a x50;3

d1 u r

r
m2 1 0:5 m2 r2
n

d x3 d1 a x50;3

7-1
7-2

The uncertainty region of the median diameter 

xm; 0 can be
calculated by the Eqs. (6) and (7).
Uncertainty region for any particle diameter can be calculated
from Eq. (7).
3.3. Total uncertainty region
In this research, the following factors are considered to calculate the total uncertainty region.
(1) Uncertainty due to sample size.
(2) Uncertainty due to measuring scale.
(3) Uncertainty due to nite dot size in a screen.
The uncertainty of measuring scale is indicated by the certication of scale measurement data. The 95% condence level of 2 lm
pitch is as follows:

dp 0:01 lm

Next, the uncertainty due to nite dot size on a screen is also

considered. It is considered that each particle size includes uncertainty region of one dot size. This value depends on the SEM magnication and the following results are obtained from the
performance data.

MBP1  10 dd 0:133 lm

9-1

MBP3  30 dd 0:40 lm

9-2

MBP10  100 dd 1:00 lm

9-3

When the SEM magnication and total dot number in a screen

are determined, the uncertainty region due to dot size is uniquely
determined. Then the values indicated in Eqs. (9-1)-(9-3) are
traceable.
The total uncertainty region of count base cumulative distribution is calculated from the following equation.

d0

q2
2
d x0 d2p d2d

10

(0)

where dx is calculated by Eq. (2).

On the other hand, the total uncertainty region of mass base
cumulative distribution is shown in the following equation.

d3

q2
2
d x3 d2p d2d

where dx(3) is calculated by Eq. (7).

11

4. The uncertainty region of MBP particles

The uncertainty region for the three kinds of MBP particles by
use of Eqs. (10) and (11) are shown in Tables 1.12.3. The uncertainty region of count and mass base cumulative distribution are
shown in Tables 1.12.3, respectively.
Figs. 3.13.3 shows cumulative size distribution based on count
and mass. The uncertainty regions are also indicated in the cumulative distribution. The uncertainty region of count base size distribution is smaller than that of the mass base size distribution. For
the count base size distribution, the uncertainty region is nearly
constant over wide range of particle diameter. But, the uncertainty
region of mass base size distribution increases as particle diameter
increases. In order to examine the reliability of uncertainty region
shown in Figs. 3.13.3, distribution of 50% count median diameter
is examined by use of experimental data.
Fig. 4.1 shows the effect of sample size on 50% count median
diameter for MBP110 particles. The upper and lower line indicate
uncertainty region calculated by Eq. (10). The uncertainty region is
nearly constant for sample size greater than about 20,000. The true
count median diameters are determined based on the data of maximum sample size and determined as follows for the three
particles.

MBP1  10 x50;0 2:86 lm

MBP3  30 x50;0 8:55 lm
MBP10  100 x50;0 21:00 lm
Figs. 4.2 and 4.3 shows the effect of sample size on 50% count
median diameter for MBP330 and MBP10100 particles, respectively. The all data is inside the uncertainty region, then reliability
of the theoretical calculated uncertainty region based on Eq. (10) is
conrmed. The effect of sample size on x10,0 and x90,0 is already
examined and it is conrmed that experimental data is inside the
theoretically calculated uncertainty region.
Fig. 5.1 shows the effect of sample size on 50% mass median
diameter for MBP110 particles. The upper and lower line indicate
the uncertainty region calculated by Eq. (11). The uncertainty

Table 1.1
Count base cumulative distribution for MBP110 particle.
x (lm)

Q0 ()

x  d0 (lm)

x + d0 (lm)

d0 (lm)

1.75
2.05
2.30
2.60
2.85
3.20
3.60
4.15
5.00

0.10
0.20
0.30
0.40
0.50
0.60
0.70
0.80
0.90

1.62
1.91
2.16
2.46
2.71
3.06
3.46
4.01
4.85

1.88
2.19
2.44
2.74
2.99
3.34
3.74
4.29
5.15

0.13
0.14
0.14
0.14
0.14
0.14
0.14
0.14
0.15

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H. Yoshida et al. / Advanced Powder Technology 25 (2014) 17481753

Table 1.2
Count base cumulative distribution for MBP330 particle.
x (lm)

Q0 ()

x  d0 (lm)

x + d0 (lm)

d0 (lm)

5.55
6.45
7.05
7.80
8.55
9.45
10.35
11.70
13.95

0.10
0.20
0.30
0.40
0.50
0.60
0.70
0.80
0.90

5.13
6.03
6.62
7.36
8.10
8.97
9.86
11.13
13.30

5.97
6.87
7.47
8.24
9.00
9.93
10.84
12.27
14.60

0.42
0.42
0.43
0.44
0.45
0.48
0.49
0.57
0.65

Fig. 3.1. Particle size distribution with uncertainty region (MBP110).

Table 1.3
Count base cumulative distribution for MBP10100 particle.
x (lm)

Q0 ()

x  d0 (lm)

x + d0 (lm)

d0 (lm)

12.00
14.50
16.50
18.50
21.00
23.50
26.50
31.00
37.50

0.10
0.20
0.30
0.40
0.50
0.60
0.70
0.80
0.90

10.93
13.42
15.38
17.32
19.77
22.18
25.13
29.46
35.63

13.07
15.58
17.62
19.68
22.23
24.82
27.87
32.54
39.37

1.07
1.08
1.12
1.18
1.23
1.32
1.37
1.54
1.87

Table 2.1
Mass base cumulative distribution for MBP110 particle.

Fig. 3.2. Particle size distribution with uncertainty region (MBP330).

x (lm)

Q3 ()

x  d3 (lm)

x + d3 (lm)

d3 (lm)

2.80
3.35
3.85
4.25
4.70
5.15
5.65
6.15
6.80

0.10
0.20
0.30
0.40
0.50
0.60
0.70
0.80
0.90

2.67
3.22
3.72
4.11
4.53
4.91
5.29
5.64
6.03

2.93
3.48
3.98
4.39
4.87
5.39
6.01
6.66
7.57

0.13
0.13
0.13
0.14
0.17
0.24
0.36
0.51
0.77

Table 2.2
Mass base cumulative distribution for MBP330 particle.
x (lm)

Q3 ()

x  d3 (lm)

x + d3 (lm)

d3 (lm)

8.10
9.45
10.70
11.90
13.10
14.60
16.10
18.20
21.00

0.10
0.20
0.30
0.40
0.50
0.60
0.70
0.80
0.90

7.70
9.05
10.27
11.39
12.44
13.68
14.79
16.25
17.88

8.50
9.85
11.13
12.41
13.76
15.52
17.41
20.10
24.12

0.40
0.40
0.43
0.51
0.66
0.92
1.31
1.95
3.12

Fig. 3.3. Particle size distribution with uncertainty region (MBP10100).

Table 2.3
Mass base cumulative distribution for MBP10100 particle.
x (lm)

Q3 ()

x  d3 (lm)

x + d3 (lm)

d3 (lm)

21.00
26.00
30.00
33.50
37.00
40.50
45.00
50.50
60.50

0.10
0.20
0.30
0.40
0.50
0.60
0.70
0.80
0.90

19.99
24.99
28.94
32.24
35.33
38.17
41.62
45.35
51.18

22.02
27.02
31.06
34.76
38.67
42.83
48.38
55.65
69.82

1.01
1.01
1.06
1.26
1.67
2.33
3.38
5.15
9.32

Fig. 4.1. Relation between 50% count median diameter and sample size for MBP1
10 particle.

region decreases as sample size increases. The true mass median

diameter and geometric standard deviation are determined based
on the data of maximum sample size and determined as follows.

MBP1  10 x50;3 4:72 lm

rg 1:348

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H. Yoshida et al. / Advanced Powder Technology 25 (2014) 17481753

Fig. 4.2. Relation between 50% count median diameter and sample size for MBP3
30 particle.

Fig. 5.2. Relation between 50% mass median diameter and sample size for MBP3
30 particle.

Fig. 4.3. Relation between 50% count median diameter and sample size for MBP10
100 particle.
Fig. 5.3. Relation between 50% mass median diameter and sample size for MBP10
100 particle.

apparatus and will be expected to use widely in various powder

handling process.
5. Conclusion
The uncertainty region of particle size distribution over all particle size range for three kinds of MBP particles is examined and
the following conclusions are obtained.

Fig. 5.1. Relation between 50% mass median diameter and sample size for MBP1
10 particle.

MBP3  30 x50;3 13:06 lm

rg 1:483

MBP10  100 x50;3 36:85 lm

rg 1:450

The uncertainty region decreases as the sample size increases. It

is also found that all the data is included inside the upper and
lower region calculated by Eq. (11).
Figs. 5.2 and 5.3 shows the effect of sample size on 50% mass
median diameter for MBP330 and MBP10100 particles, respectively. It is also found that all the data is inside the upper and lower
calculated lines, then reliability of the theoretical uncertainty
region based on Eq. (11) is also conrmed.
The effect of sample size on x10,3 and x90,3 is already examined
and it is conrmed that experimental data is inside the theoretically calculated uncertainty region.
In order to evaluate particle size distribution, the uncertainty
estimation method proposed in this research is reliable. The three
kinds of MBP particles examined in this research are considered as
suitable reference particle candidates for the size measurement

(1) The uncertainty region of count base cumulative size distribution is smaller than that of the mass base cumulative
distribution.
(2) The uncertainty region of count base cumulative distribution
is nearly constant over wide range of particle diameter and
the region is nearly constant for sample size greater than
about 20,000.
(3) The uncertainty region of mass base cumulative size distribution increases with the increase of particle diameter.
(4) The reliability of the theoretical uncertainty region used in
this research is conrmed by the experimental data of particle size measurement.

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