4.

FORMULATION OF THE RESIDENCE TIME DISTRIBUTION

4.1. RESIDENCE TIME DISTRIBUTION (RTD) MEASUREMENT

Basic radiotracer methodology includes the accurate measurement of the residence time
distribution (RTD) and its utilization for troubleshooting and diagnosis.

The principle of the RTD consists in a common impulse-response method: injection of a tracer at
the inlet of a system and recording the concentration-time curve C(t) at the outlet (Fig.24). A sharp pulse
of radioactive tracer is injected upstream of the vessel and a detector located at the inlet marks time-zero.
A second detector, located at the outlet, records the passage of the tracer from the vessel. The response of
this detector is the residence time distribution.

FIG.24. Principle of RTD method

The RTD function E(t), is represented by the equation:




E(t) = C(t)/ C t  dt
0
Where C(t) is the tracer concentration versus time at the outlet of the system. The experimental
RTD is calculated from the count rate distribution at the outlet of the system I(t), cps or cpm.

The instantaneous injection (Dirac pulse) of tracer is normally applied in practice because gives
directly the RTD, requires less tracer, is simple and rich in information. An injection is considered as
instantaneous when its duration is less than 3% of the whole mean residence time within the system.

The residence time distribution and mean residence time (MRT) are parameters that are extremely
pertinent to the operation of chemical reactors, influencing, as they do, both the throughput and the
quality of the product. Figure 25 shows an exemplary E(t) function; MRT and its standard deviation (SD)
are depicted.

MRT(τ) and SD (σ) have the following physical interpretation in relation to flow systems:
 MRT is directly related to flow rate Q and the effective flow volume V of the system: τ = V/Q,
where: V – effective volume of the system, Q – constant, volumetric flow rate.
 SD (standard deviation of MRT) characterizes the mixing rate of the given medium in the system. In
case of lack of mixing (plug flow) SD equals zero. The higher is mixing rate, the greater value of SD.
For perfect mixing system E (t) is an exponential function.

FIG.25. The exemplary E (t) function with MRT and SD parameters shown.

Fig.26 presents E (t) functions having the same MRT values but different SD that is different
mixing rates.

FIG.26. E(t) functions for different degree of backmixing.

4.2. RTD FORMULATION

The correct RTD formulation is the basic request for further data processing, modeling and
interpretation. Normally the RTD experimental data contain statistical fluctuations and other parasite
influences. Fig. 27 shows a typical experimental response in a form of discrete points.
 FIG.27. Radiotracer cloud in the screen of the data acquisition system

The main treatments (or corrections) of the experimental response curve to obtain the correct RTD
curve are the followings.

4.2.1. Dead time correction

Nearly all detector systems have a minimum amount of time that must separate two gamma
photons in order that they are recorded as two separate pulses. This minimum time delay (or dead time, )
may be due either to the physical detection process itself or to associated electronic devices.

The relation between the true nt(t) and the measured nm(t)count rate is as follows:

With a dead time of 10 s the error is less than 10% up to the fairly high value of 104 cps.

4.2.2. Background correction

Prior to the injection of radiotracer into a system, it is necessary to measure the background
radiation level, which is subtracted from the experimental data (Fig. 28).

FIG.28. Raw signal and background corrected signal

4.2.3. Radioactive decay correction

Since radioisotope tracers decay exponentially with time, it is necessary to apply decay correction
to the measured data (otherwise, more weight would unduly be given to early measurements). The decay
corrected count rate nc(t) is given as:

Where:  is the decay constant, t is the time and T½ is the half-life of the radioisotope tracer.
 The effect of the correction for the radioactive decay in radiotracer applications is illustrated in the
figure 29. The blue experimental curve in the figure 29 presents the results of the radioisotope tracing
with 113mIn (half-life 5970 s). Because of the relatively long duration of experimental measurement (1400
s) the radioactive decay correction is necessary. The real experimental curve corrected for radioactive
decay of 113mIn is shown in the same figure 29 in red color. If the decay correction is not applied, one gets
the wrong impression that the tracer concentration is decreasing at the end of experiment (blue curve
uncorrected). Applying the decay correction shows that the tracer concentration actually has reached a
constant level (red curve corrected).

FIG.29. Effect of the correction for the radioactive decay with 113mIn
4.3.4. Filtering (or smoothing)
The aim of filtering is to eliminate, or at least decrease, fluctuations due to counting statistics or
electronic noise (Fig. 30).

FIG.30. Filtering (smoothing) of fluctuations of experimental RTD curve.

Several methods for smoothing a signal are available. The Fourier transform is very effective as
many high frequencies can be filtered without altering the general shape of the experimental RTD curve.
The Fourier method requires that the data be sampled at equidistant (regular) intervals. Cumulating or
resampling counts is simpler technique for smoothing fluctuations. Counts are cumulated by groups of 5,
25 and 100.

Fig. 31 shows the typical experimental curve obtained after corrections.

FIG.31. The experimental RTD curve obtained from raw experimental data
4.2.5. Data extrapolation
Data extrapolation is needed when the end of the measured tracer curve is missed for different
reasons (large RTD, long tail, data acquisition system problems, etc). Regular tracer test assumes the
count rates go back to zero after the end of the data acquisition sequence, as illustrated in Fig. 32. Mostly
extrapolation is performed mathematically using exponential decay function.

FIG.32. Incomplete experimental curve from tracer test and its extrapolation

The aim of data extrapolation is to extend the tracer curve in some plausible way. The most
common procedure is to check that count rates decrease exponentially at the end of the experiment; this is
easily done by plotting the logarithm of count rates versus time, which should exhibit a linear behavior
towards the end. A decaying exponential function should then be adjusted on that part of the curve, and
the data extended with this function until count rates are negligibly small. The number of extrapolated
points should obviously be “reasonable” (the meaning of “reasonable” depends very much on available
data and level of precision desired).

4.2.6. Normalization of the area of experimental tracer curve

One last operation can then be performed, i.e. area normalization. This operation has several
benefits.

First of all, the influence of all the factors that affect the area of the curves but not their shape
(injected activity, radiation attenuation by walls) is eliminated. It is then possible to compare readings
from two experiments with different injected activities, or at two points with different wall thickness.

Secondly, the calculation of moments is simpler with area-normalized data. Thirdly, area-
normalized curves are in certain cases RTD curves that have a precise meaning in terms of fluid
population balance.

Area normalization is compulsory when modeling the RTD data using suitable software. The tracer
concentration curve is normalized by dividing each data point by the area under the curve (i.e. the total
count number):
 Where

 nc(t) is the corrected count rate (i.e. the result of all the previous operations),
 E t  is the normalized function.

Since count rates are actually known at discrete intervals t , values of function E t  can only be
calculated at the same intervals:

Where, nc,i is corrected count rate at time i.Δt.

The area under the new curves is therefore unity. If the tracer injection can be considered as a Dirac
pulse, function E(t) is the RTD at the measurement point. It is also customary to define the cumulative
RTD function F(t). This function can be useful when analyzing the behavior of a system:
t
F t    E u du
0