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Estimator based Flooding Predictor for (13C) Cryogenic Separation Column

C.I. Pop1, E.H. Dulf1, Cl. Festila1


Technical University of Cluj-Napoca

Department of Automatic Control
26-28 Gh. Baritiu Str., 400027 Cluj-Napoca, Romania
Abstract- The industrial distillation plants- like those for crude
oil- and the cryogenic distillation column for (13C) isotope enrichment have in common the probability to appear an undesirable
phenomenon: the flooding, when the plant efficiency decreases
drastically. After a general description of the isotope separation
problem, the paper describes the column mode of operation and
gives the mathematical equations, which explain the column flooding process. The authors deal with the online prediction methods
and propose a simple, low-cost method based on the supervision of
the process variables: differential column pressure (top-bottom)
and liquid level in boiler (variables, first and second derivatives).
Using a test-version of the column, where the flooding can be observed directly, the method proposed by the authors proves its
Keywords: (13C) cryogenic distillation, flooding, pattern recognition, prediction

Isotopes are species of the same element with different number of neutrons in the nucleus. For instance, the chemical element carbon consists of the basic species (12C) and the
heavier stable isotope (13C) with a ratio of natural concentration of (98.89% / 1.11%) [1,2]. If some chemical compounds of
carbon with higher concentration in (13C) isotope in detriment
of (12C) can be obtained, the detection of those chemical compounds brings valuable quantitative and qualitative information
in various domains: chemical engineering, biology, medicine,
A great variety of technologies able to create compounds
with higher abundance in the isotope of interest are known today. In the case of (13C) one of these is the cryogenic distillation.
The separation process analysis is based on the hydrodynamic process- specific for each separation technology- and
the separation process itself, relatively independent of the
technology used.
Unfortunately, the physical and chemical properties of the
compounds of (12C) and (13C) are very close, being difficult to
separate. Even though, very small differences in properties
must be used to raise the concentration of (13C) to separate
the isotope of interest. For instance, at very low temperatures
( 190D C ) the carbon monoxide based on (12C) has a higher

1-4244-2577-8/08/$20.00 2008 IEEE

vapor pressure (p) than the monoxide based on (13C). It is possible to find and to maintain a small range of temperature in
which the gaseous phase (related to (12C)) coexists with the
liquid phase (based on (13C)). It is necessary to distillate the
compounds (12CO versus 13CO) in a distillation column like in
the typical industrial distillation equipment [3]: the gaseous
phase must be evacuated and the liquid phase which contains
a greater abundance of 13CO - is kept as end-product. The basic
factor is the separation coefficient [1], given by the ratio
of the vapor pressures:

pD13 CO
pD12 CO



with = 1.011 , pD13 CO the vapor pressure of 13CO and pD12 CO the
vapor pressure of 12CO.
This particular isotope separation technology is called
cryogenic distillation.
The equipment is called cryogenic distillation column,
figure 1, and is divided for simplicity- in three parts [3]: the
boiler (B) on the bottom side, the condenser (C) at the top side
and the packed distillation column (tower). The external
flows are: the feed flow (F), the waste flow (W) and the product flow (P).
In the column, an upward vapor (gas) stream, generated by
the evaporation in the boiler is brought into contact with a
downward flowing stream of liquid produced by condensation
in the condenser zone. The boiler is heated with an electrical
resistor and the condenser is cooled with liquid nitrogen. During this permanent contact, the concentration of (13CO) increases in the liquid phase in the column basis. The packing material
inside the column increases the contact surface between the
liquid and the gaseous phases. In order to flow up from the
boiler to the condenser, the vapor stream needs some effective
area through the elements of the packing material. This area is
greater by dry packing material and smaller by wet material.
The gaseous upstream needs a differential pressure along the
column. Every liquid droplet is submissive to the force of gravity and, in the opposite direction, to the pressure force of the
gas. In normal mode of operation, the gravity is stronger and
the liquid phase flows as droplets to the boiler.

Figure 1. Scheme of the cryogenic distillation column

By too high differential pressure, the quantity of liquid on

the packing material increases and the column is no longer effective in washing away the undesired component from the
gas [7,8]. The gas pressure and liquid quantity impedes proper
gas transit and the liquid droplets are suspended on the packing material. This phenomenon - the flooding reduces drastically the column efficiency and can compromise the whole
process of isotope separation.
The general particularity of the isotope separation process is
the huge ratio between the feed flow-rate and the final product
flow-rate (F/P >>). An imposed column efficiency: shorter
separation time/higher isotope enrichment, leads to a higher
charge of the column: greater flow rates (F,W), more thermal
energy in boiler, etc. But the column capacity is limited and by
surpassing the certain values of operational variables, many
undesired states may occur, the most frequent being the flooding. Thus, the column operates under stress.
In normal mode of operation, the gaseous phase is assumed
to flow upward inside the numerous small channels having
the same characteristic dimensions. The liquid phase flows
down the fictious walls of the channels and reduces the
available cross-sectional area for the gas flow, thus causing a
pressure drop (a differential pressure p ). The pressure variations may be caused by other disturbances: feed material
quality/ composition, temperature distribution, flow-rates
changes, etc.
An operation of the isotope separation column with as high
as possible charge (flow rates, heating and cooling energy) is
desired, but under these circumstances, the possibility to onset
the flooding increases, with disastrous consequences. A flooding predictor, in the ideal case, will keep the column point of
operation close to the flooding (higher efficiency), but in a safe
area. If some input/ internal variables change and the flooding
can appear, the predictor alarms the operator - in open loop - or
even gives a control signal- in closed loop- to avoid future
flooding. So, the flooding predictor can be viewed as an advanced process control strategy that utilizes a pattern recog-

nition system to identify pre-flooding conditions being possible

to increase the stability and energy efficiency of the column
More methods to predict flooding onset are known today,
methods that can be divided in offline and online ones. For
instance, for packed distillation columns (also valid for isotope
separation columns) several offline empirical/ analytical flooding models exist [4]:
a. generalized pressure drop correlation (GPDC);
b. suspended-droplet models;
c. double-film models;
d. flooding velocity ( us ) prediction;
e. pressure drop correlation, etc.
For all these methods, numerous experimental data are necessary to determine the values of the main parameters. Based
on these models, the calculated and the measured values of
the variables are compared, the results being used to refine the
models. Of course, the heat losses and the apparatus indications
may be the source for differences.
The online methods use both the static and the dynamic
models of the column [5]. One supposes the availability of the
measurements of differential pressure ( pk ), liquid level in
the boiler ( h B ), feed flow rate ( Fk ), etc and it is possible to
calculate (online, using the process computer) their derivatives:
p , h B , etc) in order to ensure the predictive capability
( p , 
of the model. The structure of the static column model able to
give the predicted differential pressure ( p ) with the prediction horizon of (k) is given in figure 2. The efficiency of the
prediction may be evaluated using the correlation factor (R),
well known in stochastic system analysis.
Dynamic models use the current inputs and their derivatives
and the past values of the main variables (like p ) to predict
the output ( p ) at (t+k).
Figure 3 gives the dynamic model principle of implementation for ( p ), using one-step and m-step time delay.

Figure 2. Static column model principle

Figure 4. Improved predicted value for differential pressure


Figure 3. Dynamic column model principle

In order to improve the prediction, the actual output (differential pressure p ) is compared with the predicted value p(t + k ) . The measured value p(t ) , filtered by
H 1 (s ) (low pass filter) is compared with the estimated value y (t ) . The prediction error, (t ) , smoothed by H 2 ( s) , is
added to the predicted value p(t + k ) in order to obtain the

improved value p(t + k ) , as shown in figure 4.



If (t ) is the flow rate of the gaseous phase for carbon monoxide and ( Rh ) is the hydrodynamic resistance, in a simplified version one supposes that:
k el Pel


1 / Rh = a b Pel



Pel (p.u.)
p (p.u.)

b3 4
b2 3
b 2
= el Pel + k el
Pel =
Pel + k el
Pel + k el
= a1 Pel + a 2 Pel2 + a3 Pel3 + a 4 Pel4


Based on some experimental data [1,2] by nominal feed

flow rate, the differential pressure ( p ) for different values of
the electrical power ( Pel ) is given in table 1.







a1 = 1.48 ; a2 = 0.23 ; a3 = 3.63 10 3 ; a 4 = 1.73 10 5

If the derivative ( p / Pel ) would be available, results:
D p ( Pel ) = 1.48 + 0.46 Pel 1.09 10 2 Pel2 +
+ 6.92 10 5 Pel3
The technical solution of the column permits to detect the
flooding and this was observed by Pel 85( p.u.) .
The measured pressure evolution and the values obtained by
interpolation are given in figure 5. The evolution of the derivative ( p / Pel ) is given in figure 6. It is not difficult to observe three different slopes:
(p / Pel )1 = 0.0834
(p / Pel ) 2 = 0.0582 (normal mode)

(p / Pel ) 3 = 0.331 (flooding)

measured values
interpolation polynomial
Differential pressure (p.u.)

k el Pel
b 2 2 b 3 3
k el +
Pel +
Pel +
Pel Pel =
a a2

a b Pel


By polynomial interpolation, with fourth order approximation, the following values of the coefficients are obtained:

where ( Pel ) is the electrical power dissipated in boiler and

( k el , a, b ) are proper coefficients. Using the long division method, the pressure drop is given by: the equation:
p =








Electrical power (p.u.)




Fig 5. Measured differential pressure evolution and the interpolation polynomial

Comparing the normal mode of operation with the flooding,

the slope of the derivative has a much greater value:
0.331 >> 0.0582

In the particular case of the cryogenic isotope separation

column, the flooding phenomenon may be predicted by the
supervision of the slope ( dp / dPel ) using the differential
(p) k and (Pel ) k .
The simplified algorithm is given by the following set of equations:
pk pk 1
Pel , k Pel ,k 1

= p k p k 1
Pel , k Pel ,k 1
< (D)


Equations (6)-(9) are implemented in the structure given in

figure 7.

The disastrous consequences of the flooding phenomenon in
distillation column justify the theoretical and practical effort of
the specialists in order to predict/avoid this process. The general solution, at least according to actual references, is the predictive control theory and methods. In the particular case of the
cryogenic distillation for (13C) separation, where the information for the temperature distribution in the column is not available, accurate and prompt information about the differential
column pressure using commercially available transducers and
about the liquid level in the boiler, using a patented modern
transducer [6], the evolution of the first and second derivative
of these variables can predict and avoid the column flooding.
The solution is modern, effective and low-cost.
The authors acknowledge the support of the Romanian National Education and Research Ministery under PN2 Grant


Figure 6. Evolution of the differential pressure derivative

Figure 7. Flooding predictor based on estimation of the differential

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