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Metrological performances of Mass Flow Controllers for dynamic gas dilution

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DOI: 10.1007/s00769-013-0974-y

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Metrological performances of mass flow
controllers for dynamic gas dilution

A. Demichelis, G. Sassi & M. P. Sassi

Accreditation and Quality Assurance

Journal for Quality, Comparability and
Reliability in Chemical Measurement

ISSN 0949-1775
Volume 18
Number 3

Accred Qual Assur (2013) 18:181-186

DOI 10.1007/s00769-013-0974-y

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 Author's personal copy
Accred Qual Assur (2013) 18:181–186
DOI 10.1007/s00769-013-0974-y
GENERAL PAPER
Metrological performances of mass flow controllers for dynamic
gas dilution
A. Demichelis • G. Sassi • M. P. Sassi
Received: 7 June 2012 / Accepted: 13 March 2013 / Published online: 24 March 2013
Ó Springer-Verlag Berlin Heidelberg 2013
Abstract The method of dynamically generating refer-
ence mixtures of volatile organic compounds at trace levels
requires the uninterrupted blending of the component flows
during the generation time. The target flow rate uncertainty
depends on the application and the range of the concen-
tration generated. Accurate air flow rates used for dilution
can be realized by mass flow controllers (MFCs). The
short-term stability of MFCs has been measured in order to
assess their usefulness in dynamic gas dilutors. As shown
here, MFCs are appropriate for the dynamic preparation of
diluted gas mixtures provided they are calibrated prior to
each use, because their calibration is not stable over longer
time periods. The calibration results of the low pressure
drop MFC proved its applicability in a wide range of
pressure drop. The uncertainty of the dilution flow rate
resulted mainly from the limited short-term stability of the
MFC at low dilution flow rate or at short generation time.
Consequently, MFCs can provide highly accurate dilution
air flow rates with a relative uncertainty of 0.2 %, for flow
rates larger than 70 % of the MFC’s maximum flow rate
and generation times longer than 5 min.
Keywords Mass flow controllers  VOC  Dynamic
dilutor  Reference gas mixture
A. Demichelis (&)  G. Sassi  M. P. Sassi
Istituto Nazionale di Ricerca Metrologica (INRIM), Turin, Italy
e-mail: a.demichelis@inrim.it
G. Sassi
Dipartimento di Scienza Applicata e Tecnologia,
Politecnico di Torino, Turin, Italy
Introduction
The method of dynamically generating reference mixtures
of volatile organic compounds (VOCs) at trace levels
requires the uninterrupted blending of the components, i.e.,
the mass flows of VOCs and dilution air [1] during the
dilution time that generally is shorter than 1 h. Different
schemes of dilutors can be adopted, diluting the VOC flow
by one or two separate, yet interfaced stages. The dilutor
scheme used in the INRIM laboratory is schematically
shown in Fig. 1: F1 and F2 are the two main dilution air
flows and Fint is the interface flow between the stages.
To make the Fint control system work properly, a pres-
sure drop from the first stage to the second one is
necessary. If diffusion tubes [2] are employed, the pressure
in the first line (p1 in Fig. 1) must be the lowest possible
and cannot exceed 10 kPa. Consequently, a low pressure
drop (2–3 kPa) flow control system must be used for the
inter-stage flow Fint.
The contribution of the air flow rates to the uncertainty
of the VOC concentration can be considered as insignifi-
cant or negligible if their significance index [3], i.e., the
ratio between the flow rate contribution and the maximal
contribution among the influence parameters in the uncer-
tainty budget is lower than 10 or 1 %, respectively. This is
related to the pre-defined target uncertainty of the VOC
concentration, which in turn limits the acceptable uncer-
tainty of the airflow rates. As a significance index of 10 %
indicates an insignificant contribution to the uncertainty
budget [3, 4], the target uncertainty of the air flow rate can
be calculated from the uncertainty budget of the generated
VOC concentration. The resulting target standard uncer-
tainty for the air flow rate is 0.2 % if the temperature of the
dynamic source is controlled to 0.1 K, or 0.1 % when
controlling the temperature to 0.01 K [3].
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182
p1
VOC
source
F1
Purified air
401325 Pa
F2
Fig. 1 Dynamic dilutor scheme. F1 and F2 are the two main dilution air flows, Fint is the interface flow between the stages, p1 is the mixture
pressure in the 1st dilution stage
Two types of devices can provide reliable air flow rates
in a scheme as reported in Fig. 1: (1) devices such as the
mass flow controller (MFC) allowing to adjust the flow rate
[5–7] and (2) fixed flow elements, e.g., sonic nozzles [8, 9].
The flow rate accuracy of the first type is generally limited
by its stability [10, 11]. Thus, an in-depth understanding of
the MFC calibration uncertainty and their short-term sta-
bility is required to use them in dynamic dilutors.
In the CCQM-K26b comparison [12], dynamic gas
standards have been prepared by permeation employing
different flow control systems in gas dilution. An expanded
flow rate uncertainty (k = 2) of 0.5 % has been calculated
for a sonic nozzle (FMI laboratory) and a standard uncer-
tainty of 0.1 % for an MFC when being calibrated against a
Brooks Vol-U-Meter (NMi, Netherlands). For a high-
accuracy and variable gas flow dilutor using MFCs, a
typical expanded uncertainty of 0.4 % has been reported in
[13].
This paper investigates into the performances of MFC:
the calibration uncertainty (with emphasis on very low
pressure drops), the variation of the calibration bias over
time, and the quantification of the short-term stability.
The scope of this work is to experimentally verify the
usefulness of MFCs in dynamic gas dilutors. The results
will lead to a more robust value than commonly reported,
for the MFC flow rate stability. It can be determinant in the
choice of the gas control system. Furthermore, the inves-
tigation into the range of lowest gas pressure in the first
dilution line contributes to optimizing the dilutor geometry,
thus allowing to miniaturize the VOC generation system.
Materials and methods
Two thermal MFCs (model EL-FLOW SelectÒ, F201CV-
20 K-AAD-33-V, Bronkhorst HI-TEC, Ruurlo (NL)) at a
nominal flow rate of 25 l min-1 under Standard condition
(273.15 K and 101325 Pa) have been tested for F1 and F2.
A mass flow controller at a nominal flow rate of
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Accred Qual Assur (2013) 18:181–186
p1 regulating
valve
p1 1-stage diluted VOC mixture
Atmospheric pressure
Fint
2-stage diluted VOC mixture
Atmospheric pressure
100 ml min-1 under Standard condition (model LOW-Dp-
FLOW, F-101D-100-AAD-33-V ? F-004-AC-LU-33-V,
Bronkhorst HI-TEC, Ruurlo (NL)) has been tested for Fint.
Hereafter, they are referred to as F25A, F25B, and F01,
respectively. According to Bronkhorst specifications, the
optimum gas inlet pressure range is 200–300 kPa above
ambient pressure for F25A and F25B, and 2–3 kPa above
ambient pressure for F01. Cylinders of synthetic air (Air
Liquide, air Alphagaz 1) with a declared purity of
99.999 % have been used without gas filter. The MFCs are
intended to be used in the INRIM dynamic dilutors for
reference mixtures for environmental studies at which in-
house generated purified air with a measured dew point
lower than 213.15 K and particles with diameters of less
than 0.01 lm only was applied.
Flow rate measurements have been performed with both
the INRIM bell prover (160 l nominal capacity,
0.2–400 l min-1) [14] and the INRIM piston prover (3 l
nominal capacity, and a nominal flow range of
0.1 ml min-1 to 2 l min-1) [15]. The experimental cali-
bration setup is reported in Fig. 2. The setup has been
tested before and after each measurement for leakages to be
lower than 10 ll min-1.
F25A and F25B have been calibrated at 10, 50, and 90 %
of their maximum flow rate by the bell prover (denoted in
Fig. 2 by number 4) with a relative calibration standard
uncertainty of 0.1 %. F01 has been calibrated at 20, 60, 80,
and 100 % of maximum flow rate by the piston prover
(denoted in Fig. 2 by number 5) with a relative calibration
standard uncertainty of 0.05 %. The calibrations have been
repeated over a period of 16 months since shipping to
evaluate the calibration bias over time. F01 has been cali-
brated at maximum flow rate at a pressure drop range from
80 to 4500 Pa. The pressure drop has been changed varying
the upstream MFC pressure (effected by valve 3 in Fig. 2)
and keeping a constant downstream pressure (atmospheric
pressure) as the dilutor configuration requires (Fig. 1).
For the quantification of the short-term stability, F25A
and F01 flow rates have been measured over 5 h as average
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Accred Qual Assur (2013) 18:181–186 183

Fig. 2 Experimental setup for

PIC FIC
MFC calibration. 1 pure air
cylinder, 2 pressure reducer set FIR
at 401325 Pa, 3 p1 regulating n.1
valve, n.1 connected for bell
prover measures, n.2 connected
for piston prover measures, 4 2 F25A – F25B n.2 4
bell prover, 5 piston prover, 6
vent to atmospheric pressure, 6
PIC pressure indication and PIC FIC
control, FIC flow rate indication 1 FIR
and control, FIR flow rate
indication and registration, DPI
differential pressure indication
3 p1 F01 5
6 ΔPI 6

values of 10 s each. Flow rates of 10, 50, and 90 % of the

maximum were studied with F25A, while for F01 just the
maximum flow rate was applied. The flow rate data were
grouped in time intervals to model observation times s
between 20 s and 100 min, thus dividing the total of 5 h
into 900 to 3 intervals containing 3 to 900 average flow rate
values, respectively. In each interval, the relative standard
deviation sr of flow rate values was evaluated. As a con-
sequence for s = 1 min, there will be 300 values of sr. For
each observation time s, the 98th percentile of the normal
distribution of the sr data was calculated, i.e., the mean
value of sr data plus 2 times relative standard deviation of sr
data. This value has been demonstrated to be a more robust
estimator than the observed maximum value of sr data [3]
for the estimation of the short-term stability.
Fig. 3 F25A and F25B relative calibration bias over time. F25B
points are circled by the gray ellipses. Dotted lines refer to the target
Results and discussion flow rate standard uncertainty (0.2 %)

Calibration bias over time

Taking the calibration flow rate of a MFC at the shipping
time, Ft0, as reference value, the flow rate Ft, measured
according to the INRIM calibration procedure at a later
time, t, can be used to calculate a relative calibration bias B
 
Fi  Ft0
B¼ ð1Þ
Ft0
B has been measured repeatedly over a 16-month period.
In Fig. 3, B values for F25A and F25B at 10, 50, and
90 % of maximum flow rate are reported as a function of
the time t. Shipping time has been set as t = 0. Each value
is the average of 4 measurements, the measurement
repeatability standard deviation is lower than 0.04 %, and
the INRIM calibration uncertainty is 0.1 % for F25A and
F25B (vertical error bars in Fig. 3). The uncertainty stated
in the manufacture’s calibration certificate for F25A and
F25B is 1 % at maximum flow [10].
In the 16-month period, a calibration bias of up to 2.5
was observed, for measurements at 10–90 % of the maxi-
mum flow rate it exceeded the target flow rate uncertainty
(0.2 %) already after a few months. The calibration bias
remained below the target uncertainty over the test period
when a MFC was operated at 50 % of maximum flow rate;
however, this hold just partly for the other tested MFC
which deviated beyond the manufacturers stated uncer-
tainty (1 %) after a year. Similar results have been obtained
for F01. Since the calibration bias exceed the target flow
rate uncertainty, a MFC must be calibrated before (and
after) each mixture generation.

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184
Fig. 4 Pressure drop Dp effect on F01 calibration standard uncer-
tainty at the maximum flow rate. The vertical error bars indicate the
standard calibration uncertainty of 0.05 % of the INRIM standard
Low pressure drop effects
A working pressure drop Dp between 2 and 3 kPa is rec-
ommended for the MFC F01 by the manufacturer. Since
the VOC source, i.e., the diffusion cell, is directly con-
nected to the first stage of the dilutor, it is opportune to
limit its pressure in order to reduce gas leakage problems
and inaccurate pressure correction for the diffusion rate.
F01 has been calibrated at different values of Dp from 80 to
4500 Pa. In Fig. 4, experimental results are shown: each
point is calculated as the average of four measurements, the
mean value of the flow rate over the tested pressure drop
range is reported as a horizontal line, the vertical error bars
indicate the standard calibration uncertainty of 0.05 % of
the INRIM standard.
Figure 4 outlines that the flow rate values vary within
the calibration standard uncertainty of 0.05 % for a pres-
sure drop between 100 and 4500 Pa. The Fisher statistical
test on experimental data of Fig. 4 outside and inside the
recommended range of 2000–3000 Pa has shown that the
experimental results belong to the same population with a
confidence greater than 97 %.
A deviation of 2.5 % from the average value of flow rate
over the pressure drop range from 100 to 4500 Pa was mea-
sured for the mass flow rate at a pressure drop of 80 Pa. It can
be summarized that above 100 Pa, even outside of the sug-
gested working range (2–3 kPa), the performance variation of
F01 is lower than the measurement uncertainty. Conse-
quently, the pressure drop has no effect on the calibration
standard uncertainty of F01 for a Dp higher than 100 Pa.
Short-term stability
The MFC short-term stability, V, has been calculated as
the 98th percentile of the normal distribution of the
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Accred Qual Assur (2013) 18:181–186
Fig. 5 Frequency of the experimental relative standard deviation sr of
the MFC flow rates at different observation times s (F25A at 90 % of
maximum flow rate). The y-axis reports the frequency of the event
normalized by the total number of events
relative standard deviation data of flow rate sr at any
given observation time s. The distribution of the sr data
is reported in Fig. 5 for the flow rate measurements of
F25A at 90 % of its maximum flow rate, for different s.
The shape of the distribution depends on the observation
time s. For s longer than 1.5 min, i.e., with more than 9
data per interval, a symmetrical shape is observed and a
normal distribution can be assumed with sufficient
accuracy.
In Fig. 6, the short-term stability V is reported in
dependence of the observation time s, at different mass
flow rates (10, 50, and 90 % of maximum flow rate for
F25A and at maximum flow rate for F01). The few data per
interval at observation times lower than 1 min might result
in a weak estimation of the short-term stability V. How-
ever, the dynamic generation of a reference VOC mixture
generally requires more than 10 min.
V slightly decreases with s for all the MFCs for all flow
rates. Thus, long observation times improve mass flow rate
stability. This aids in the identification of the optimum
observation time for any generation of dynamic gas mix-
tures, e.g., the sampling time for a canister or the residence
time for flowing in a spectroscopic cell.
The best flow rate stability V has been observed at
maximum flow rate while it approaches 3 % at 10 % of
maximum flow rate. The analysis of V data for F25A
shown in Fig. 6 has revealed a logarithmic dependency on
the observation time s and mass flow rate F. The best
fitting result is reported as Eq. 2.
ln V ¼ ð0:11 F  0:199Þ ln s  3:894 F  3:262 ð2Þ
where V is the flow rate stability, s* is the numerical value
of the observation time when expressed in min and F is the
fraction of the actual flow rate under Standard conditions
relative to the maximum flow rate.
 Author's personal copy
Accred Qual Assur (2013) 18:181–186
Fig. 6 MFC short-term stability versus the MFC observation time s
for F25A and F01 at different percentages of maximum flow rate
The nominal maximum flow rate of F01 is lower than
10 % of the F25A maximum flow rate. Nevertheless, F01
has shown a better short-term stability, i.e., around 0.2 %
versus the 2 % of F25A at 10 % of maximum flow rate.
This may be due to the valve geometry, to the inherent
characteristic curve, and to the different ranges of the grade
of opening at which the valves operate.
The flow rate stability of F25A is better than the target
standard uncertainty for the flow rate of 0.1 % or 0.2 %
only for high flow rates. The short-term stability of F25B
has been considered in this work close to that of F25A, due
to the same valve geometry.
Flow rate combined uncertainty
The combined uncertainty of the flow rate has been cal-
culated as the combination of the calibration standard
uncertainty and the short-term stability at different obser-
vation times. Following the ISO/IEC Guide 98 (generally
known as GUM) [16], the contributions can be combined
Fig. 7 Flow rate combined
standard uncertainty
u(F) (curved surface) versus the
MFC flow rate F and
observation time s. The
horizontal plateau is the target
flow rate standard uncertainty of
0.2 %. Data are reported for
F25A
20
40
60
Observation time,
τ (min)
185
as their quadratic sum. As previously discussed, no pres-
sure effect on the flow rate calibration standard uncertainty
has been considered.
The calibration standard uncertainty has been derived
from the traceable MFC calibration. To eliminate the
contribution of the calibration bias, it has been suggested to
calibrate the instrument before each use. The calibration
standard uncertainty gives a constant contribution on the
whole F and s ranges, while the short-term stability gives a
variable contribution expressed by Eq. 2. In Fig. 7, the
mass flow rate combined standard uncertainty u(F) is
reported as a function of the observation time s and of the
mass flow rate F for F25A (the curved surface). Expressing
the mass flow rate F by the percentage of its maximum
provides a direct comparison among MFCs of other span
but with the same control valve.
The evaluated uncertainty for the flow rate is strongly
dependent on F (percentage of maximum flow rate) and on
the observation time at low flow rates. Figure 7 reflects the
behavior of the short-term stability which represents the
dominant contribution to the flow rate combined standard
uncertainty. The horizontal plateau refers to the target flow
rate standard uncertainty of 0.2 %. As a result, the com-
bined uncertainty of the flow rate is lower than the target
standard uncertainty only for high flow rates, i.e., on the
left side of Fig. 7. It follows that the target dilution flow
rate uncertainty can be guaranteed working with the MFC
at flow rates larger than 70 % of its maximum flow rate and
for observation times longer than 5 min.
Conclusion
In this paper, MFC performances have been experimentally
analyzed to investigate their use in dynamic gas dilutors.
2.0
1.5
Flow rate
1.0 standard
uncertainty,
u(F) (%)
0.5
0.0
20
40
60
80 80 Flow rate, F (%)
(percentage of maximum flow)
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186
The following MFC conditioning procedure was employed:
instrument warm up time of at least 1 h with the set flow
rate flushing before measurements, using purified air (dew
point lower than 213.15 K and particle diameters of less
than 0.01 lm), laboratory temperature control better than
1 °C, ambient atmospheric pressure, and 30–70 % relative
humidity.
Experimental evidence has been given to the fact that
MFCs need to be re-calibrated before and after each use to
guarantee the uncertainty requirement for the generation of
reference VOC mixtures. This suggests to provide a
handheld flow rate transfer standard that can be used before
each generation. Alternatively, gas control systems based
on fixed flow elements can be employed due to the easier
calibration procedure.
No systematic pressure effect was found to act on the
provided standard uncertainty of mass flow rate calibration
for the low pressure drop MFCs, in an inlet pressure range
from 100 to 4500 Pa. Consequently, it will be possible to
construct a dilutor with a pressure limit in the first dilution
stage down to 100 Pa which does not perturb the VOC
mass flow rate from the generator. This allows to minia-
turize the VOC generation system with a low designed
pressure loss.
A method for a conservative evaluation of the MFC
short-term stability over time (1–100 min) has been pro-
posed. The MFC short-term stability was found to be
strongly flow rate-dependent and time-dependent at lower
flow rates. As a consequence, the MFC flow rate accuracy
is limited by the flow rate short-term stability at lower flow
rates. It is pointed out that the longer the observation time,
the better the MFC stability, granting better concentration
stability when a generated gas mixture is sampled for a
longer time in a canister or in a detector cell.
In conclusion, the target standard uncertainties of
0.1–0.2 % for flow rates can be guaranteed using MFC in
dynamic dilutors provided the flow rate control systems are
calibrated before each mixture generation with the pro-
posed conditioning procedure, employing a flow rate of
more than 70 % of the maximum and a generation time
longer than 5 min. Otherwise, dynamic dilution systems
need to be based on more stable flow rate control systems,
e.g., fixed flow elements.
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Accred Qual Assur (2013) 18:181–186
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