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Article history: Optical thermometry offers great precision, repeatability, flexibility, and stability, hence pro-
Received 26 August 2019 viding performance advantages in non-contact temperature measurement. To assess its
Received in revised form 8 October potential for controlling the temperature of steam cracking furnaces, ethane steam cracking
2019 experiments were carried out on pilot plant scale. The control performance of the pyrome-
Accepted 14 October 2019 ter was found to be comparable to that of a weld-on type K thermocouple, the latter being
Available online 24 October 2019 representative of the industrial standard. The tested optical thermometer is suited as a sen-
sor to measure tube metal temperatures of a steam cracking reactor coil, either inside or
Keywords: outside of the firebox. Due to its fast response time, optical thermometer temperature mea-
Steam cracking surements help to prevent temperature overshoots, which have an adverse effect on the
Pyrometry tube longevity and coke formation. Flexibility in positioning makes optical thermometry a
Optical temperature measurement viable alternative compared to conventional type K thermocouples.
Furnace control © 2019 Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
Pilot plant
Fig. 1 – Diagram of the optical thermometer, focusing on the components that convert the electromagnetic radiation to an
interpretable digital or analog signal.
range. However, thermocouples experience an inherent drift ima and averages in a specified time interval. The precision of
caused by metallurgical changes over time during oper- the temperature measurement is determined by the amount
ation (Bentley, 1990). Even more important for industrial of electrical noise in the probe head. The described combina-
and pilot plant scale is that once experimental failure of tion of parts allows to detect temperature changes as small
the thermocouple occurs, the entire plant has to be shut as 0.01 K. Up to 1000 measurements per second are possible,
down for repair works. Movable non-contact temperature with a thermal drift of less than 0.1 K per year. When rigorously
measurement devices might in this case offer a worthy alter- calibrated, the accuracy of the measurements is within 1.5 K.
native. Given its high measurement accuracy, fast response and low
thermal drift, the temperature measurements of a pyrometer
2.1.2. Optical thermometer could not only be used for furnace firing control, but also as
The pyrometer consists of several components that convert an input variable for calibration or tuning of a process model.
the electromagnetic radiation emitted by a surface to a digital The latter could in turn assist process operators in optimizing
signal that can be interpreted by a computer or to an ana- the startup, shutdown and operational procedures of steam
log signal that can be used as input to a programmable logic cracking furnaces, thus increasing the energy efficiency and
controller (PLC), see Fig. 1. reducing the emissions to the environment.
The collection optics receive electromagnetic radiation
emitted by a surface. A combination of lenses and in some 2.2. Pilot plant for steam cracking
cases flexible fiber optic cables captures the radiation from a
small focal point on the target surface and conveys it to the A schematic representation of the pilot plant for steam crack-
electronic components in the probe head. Installing a fiber ing is given in Fig. 2. As a detailed description of the unit, the
optic cable between the collection optics and the probe head analytical equipment and the calibration procedure is avail-
has the advantage that the electronic components of the probe able elsewhere (Dierickx et al., 1986; Vandamme and Froment,
head can be located sufficiently far away from the furnace in 1982), only a brief description is given, based on Wang et al.
order to not interfere with the strict zoning regulations that (2007), Dhuyvetter et al. (2001) and Van Geem et al. (2010).
are enforced on petrochemical sites. However, the downside The feed section controls the supply of different feedstocks
is a lower signal-to-noise ratio as up to 80% of the light can to the reactor coil. The feedstock can be gaseous (ethane,
be attenuated by the fiber optic cable. In that case, in-place propane, butane), liquid (hexane, naphtha, gas condensate,
calibration is required to obtain a correct absolute tempera- etc.) or solid (e.g. waxes). The mass flow rate of liquid hydro-
ture measurement. The first signal processing step is to isolate carbons and water is set using a CORI-FLOW mass flowmeter
the desired wavelength from the incoming light. Two options controlled pump. The flow rate is automatically regulated by
are available: electromagnetic radiation with a wavelength of adjusting the pumping frequency of the pump. The furnace,
1600 nm is used to measure temperatures between 400 K and built with silica/alumina bricks (PROMATON® ), is 4.0 m long,
3075 K while radiation with a wavelength of 900 nm is used to 0.7 m wide and 2.6 m high. The power is supplied via ninety
measure temperatures between 600 K and 3275 K. Those two premixed gas burners, equipped with automatic fire checks
wavelength options are selected to minimize the interference and arranged on the side walls to provide a uniform heat dis-
with optically active molecules commonly present in air or tribution over the height of the furnace.
in flue gas from natural gas combustion (H2 O, CO2 , CO, CH4 , The furnace is divided into seven separate cells, which can
etc.). The photons of the selected wavelength are converted be fired independently to set any type of industrially relevant
to an electrical signal in a solid-state photodetector made of temperature or heat flux profile over the length of the reactor
silicon or an indium gallium arsenide (InGaAs) ternary alloy. (Van Geem et al., 2010). The firing rate is controlled in each
The amplifier strengthens the signal from the photodetector cell by adjusting the pressure in the premixed fuel feed line
to allow currents as low as 10−15 A to be detected. The con- to the burners. Twenty thermocouples and five manometers
tinuous electrical signal is discretized by an analog to digital are located along the reactor coil to measure the tempera-
convertor and the discretized signal is supplied to the proces- ture and pressure of the process gas as indicated in Fig. 2.
sor unit which calculates the surface temperature based on The reaction section of the tube is made of Incoloy 800 H T
the intensity of the discretized signal. The temperature sig- and is about 12 m long with an internal diameter of 9 × 10−3
nal can be digitally interpreted via dedicated software but can m. The tube is designed to achieve turbulent flow conditions
also be supplied directly to a PLC system via a 4–20 mA signal (Re > 7000) in the coil with reasonable feed flow rates (∼10−3
or a 0–10 V output. Basic signal processing can be carried out kg/s of hydrocarbons). The pressure at the exit of the reac-
by the processor to filter outliers and to provide minima, max- tor is controlled by a reduction valve. At the reactor outlet,
Chemical Engineering Research and Design 1 5 3 ( 2 0 2 0 ) 380–390 383
Fig. 2 – Schematic overview of the pilot plant setup, indicating the most important temperature (o) and pressure
measurements (P) (1: electronic balance, 2: demineralized water reservoir, 3: liquid hydrocarbons reservoir, 4: heated
sampling oven (570 K), 5: heated transfer lines (570 K), 6: oil cooled heat exchanger, 7: water cooled condenser, 8: cyclone, 9:
thermal mass flow controller (internal standard addition), 10: outlet pressure regulation valve, 11: water cooled heat
exchanger, 12: dehydrator). The location of PYRO 3, TK 1 and PYRO 1 at the outlet of cell 7 is highlighted in color (Van Geem
et al., 2010).
the injection of nitrogen provides an internal standard and ted around the reactor outlet section, where the reactor exits
contributes to a certain extent to the quenching of the hot through the furnace wall. To avoid damage to the lenses, the
reactor effluent. Before the cooling of the effluent, a sample is temperature of the optics should be kept below 330 K. Hence,
taken for the on-line C5 + analysis, performed using compre- mounting a light pipe or a lens directly inside the furnace
hensive two-dimensional gas chromatography (GC × GC) (Van was not possible. However, a custom collar fitted around the
Geem et al., 2010). After cooling, another sample is drawn from reactor outlet was designed to minimize heat losses and to
the product gas for on-line C4 - analysis via one-dimensional maximize the responsiveness by having a low thermal heat
gas chromatography (GC). During the decoking of the reactor capacity and low thermal conductivity.
coil, the mass of coke deposited in the reactor is measured Fig. 3 illustrates the design of the custom collar fitted
through the gasification products CO and CO2 . Via a combina- around the reactor outlet section as well as its actual posi-
tion of a volumetric flow meter and an infrared analyser for CO tion. The first two pyrometers were mounted on the custom
and CO2 , the mass of deposited coke can be calculated based collar, 0.038 m apart to check consistency, but only one was
on a straightforward carbon balance and applying the ideal used for control purposes during the experiments. The pri-
gas law. This is illustrated Eq. (1). In this equation, MMC is the mary pyrometer is referred to as PYRO 1 while the secondary
molar mass of carbon, T is the temperature, p is the absolute pyrometer is referred to as PYRO 2. A type K thermocouple was
pressure, V is the volumetric flow rate, ϕCO and ϕCO2 are the welded to the reactor outlet in between the furnace brick wall
CO and CO2 volume fractions in the effluent measured via the and the custom collar. This weld-on thermocouple measur-
infrared analyser and t is the time between subsequent mea- ing the tube metal surface temperature provided the required
surements. The index i relates to the discrete measurements validation data for the optical thermometers positioned on
at the sampling frequency 1/t. the reactor outlet. This thermocouple is referred to as TK 1. A
third pyrometer was positioned outside the furnace and was
MMC V p used to collect infrared radiation through an opening in the
i i
mcoke = ϕCO,i + ϕCO2 ,i t (1)
R Ti refractory from a small focal point on the outlet bend of the
i
reactor in the last cell of the furnace, i.e. cell 7. This pyrometer
is referred to as PYRO 3. At the same axial position, a type K
2.3. Installation of pyrometer in the pilot plant
thermocouple inside a thermowell measured the process gas
temperature.
In the default situation, the various temperature measure-
So the optical measurement of the tube metal temperature
ments in the pilot plant are carried out using type K
could be compared with the process gas temperature mea-
thermocouples in thermowells protruding in the reactor coil
surement by the type K thermocouple. This thermocouple is
to measure the process gas temperature in combination with
referred to as TK 3. Fig. 4 shows the mounting of the pyrom-
type K thermocouples that are welded on the reactor surface
eter on the outside of the furnace and provides insight in the
to measure the tube metal temperature. The pyrometers were
installed on two locations in the unit. A custom collar was fit-
384 Chemical Engineering Research and Design 1 5 3 ( 2 0 2 0 ) 380–390
Fig. 3 – (a) Design of the custom collar around the reactor outlet section to mount two pyrometers and one additional device.
(b) Fit of the custom collar around the reactor coil after exiting the furnace: CAD drawing. (c) Reactor tube without the
custom collar.
Fig. 4 – (a) Positioning of the pyrometer analyzing the tube metal temperature on the outlet bend of cell 7. (b) Focal point of
the optical temperature measurement device (digitally enhanced) with a diameter of around 0.001 m on a 0.009 m diameter
reactor.
focal point size of the lens (diameter of about 0.001 m) on the The temperature control loop is visualized in Fig. 5. The
0.009 m internal diameter reactor. regulated parameter in the studied system is the outside tube
metal temperature (TMT) which indirectly relates to the con-
version or so-called cracking severity. This corresponds to
today’s industrial standard. Different temperature measure-
2.4. Experimental procedure and data analysis
ment devices are tested sending a temperature signal, i.e.
measured process variable (PV), to the PID controller where it
Three types of experiments were carried out, differing in the
is compared to the desired set point (SP). The final control ele-
temperature measurement device to control the firing in cell
ment in the loop is a valve regulating the flow rate of premixed
7 of the furnace: PYRO 1, TK 1 and PYRO 3 were used dur-
combustion gas. By adjusting the valve opening, the flow rate
ing a 6 h cracking cycle in which the temperature set point
of premixed combustion gas to the firebox is regulated, i.e.
was changed twice to observe the performance of the temper-
manipulated variable (MV). Tuning of the PID controller, which
ature measurement in varying circumstances. The two new
is in turn integrated into the programmable logic controller
temperature set points were 10 K and 25 K higher than the
(PLC), is performed using the heuristic Ziegler-Nichols tuning
initial set point. The firing in the other cells of the furnace
method.
was controlled via the default control system throughout all
experiments.
Chemical Engineering Research and Design 1 5 3 ( 2 0 2 0 ) 380–390 385
Fig. 5 – Block diagram for the process control system. The final control element, i.e. process valve, adjusts the burner gas
flow rate, impacting the temperature measured by the temperature sensor (PYRO 3, TK 1 or PYRO 1 depending on the
experiment). The measured process variable is subtracted from the set point to compute the controller error. The PID
controller output to the process valve is based on this error.
The following experimental details were common to all pressure and flow rates were logged to have comprehen-
experiments. Ethane was used as a hydrocarbon feedstock. sive information on the state of the furnace at the moment
During cracking, 0.833 × 10−3 kg/s ethane and 0.321 × 10−3 kg/s of sampling. These snapshots of temperature and pressure
steam are fed to the reactor, resulting in a steam dilution of rather than their continuous measurements were used to
0.385 kg/kg. Each experiment started with the reactor inner draw conclusions with respect to process yields due to the dis-
surface in the oxidized state as a consequence of the decoking crete nature of the yields measurements. Error bars in figures
procedure in the previous experiment. The following exper- correspond to the 68% confidence interval equaling a single
imental procedure was adopted for all experiments, further standard deviation .
referred to as step 1 to step 8, with step 8 of the previous
experiment being equal to step 1 of the following experiment.
3. Results and discussion
1 Pre-oxidation of the reactor coil during decoking in the pre-
vious experiment. Two repetitive experiments were carried out with differ-
2 Leak test using N2 at a pressure of 4 bar during 300 s. ent temperature measurement devices (PYRO 1, TK 1 and
3 Preheating of the reactor coil using the default temperature PYRO 3) following the eight steps as described in Section 2.4,
measurement (TK 3) for control. Steam is supplied to the resulting in a total of 6 experiments. The experiments were
reactor. labelled according to the following convention: XXm–n where
4 Cracking using the default temperature measurement (TK XX indicates the temperature measurement method (PY for
3) for control during 4080 s. pyrometer-based control and TK for thermocouple-based con-
5 Cracking using the alternative temperature measurement trol), m indicates the position of the process measurement (1
(PYRO 1, TK 1 or PYRO 3) for control during 6600 s at the refers to the measurement outside the furnace and 3 refers
equivalent temperature set point of step 4. The equivalent to the measurement inside the furnace, as shown in Fig. 2)
temperature set point is determined as the stable value of and n is used to differentiate between the two experiments
the alternative temperature measurement during step 4. performed with the same temperature measurement device.
6 Cracking using the alternative temperature measurement For example, PY3-1 is the first experiment carried out with
(PYRO 1, TK 1 or PYRO 3) for control during 5160 s with a set the pyrometer collecting radiation from the outlet bend of the
point 10 K higher than the set point of step 5. reactor inside the furnace, PY3-2 corresponds to the repeat
7 Cracking using the alternative temperature measurement experiment with the same temperature detector on the same
(PYRO 1, TK 1 or PYRO 3) for control during 5760 s with a set location. All experiments were carried out according to the
point 25 K higher than the set point of step 5. stepwise procedure described in Section 2.1. To guarantee that
8 Decoking of the reactor via gasification with a steam/air all experimental data is gathered at comparable conditions,
mixture, including pre-oxidation of the reactor for the next the preheating and initial cracking, corresponding to step 1–4,
experiment. is performed with the default thermocouple TK 1. Only when
the system is stable, the alternative temperature measure-
Effluent composition analyses are done consecutively, as ment device (PYRO 1, TK 1 or PYRO 3) is added as detector in
frequently as the gas chromatography allows. The C4 − anal- the control loop. The performance of each of the control sys-
ysis takes approximately 1500 s, a new sample injection is tems in terms of stability, precision and reproducibility was
started once the previous C4 − analysis cycle is finished. This investigated for the following three aspects: temperature and
implies that two to three C4 − analyses can be done per pressure, product yields and coke formation.
step during steps 4–7. The most abundant components were The main focus of the present work is on the performance
the unconverted feed component (ethane), the correspond- of the pyrometer as a temperature measurement device in a
ing olefin (ethene) and the light components (hydrogen gas, PID control loop, in particular with respect to yields and coke
methane). Other C4 − components were measured but their formation. The dynamic behavior of the system with respect
yield was generally small (<2 wt.% in total). The focus in the to temperature will be studied in detail in Section 3.1 since
current campaign is on the C4 − analysis as only a small frac- the temperature will impact the product yields and both the
tion of the reactor effluent in ethane cracking has a carbon amount and the nature of the formed coke. Therefore, Sec-
number higher than 4 at the cracking severity targeted in tions 3.2 and 3.3 aim to provide a thorough analysis of the link
the present experiments. At the moment of injection of the between the temperature measurements and the product and
sample to the GC, all available measurements of temperature, coke yields, respectively.
386 Chemical Engineering Research and Design 1 5 3 ( 2 0 2 0 ) 380–390
3.1. Temperature and pressure value as in step 4. Only PY3-n succeeds in keeping the tem-
perature more or less constant while PY1-n and TK1-n appear
Temperatures measured during experiment PY3-1 using PYRO to show a drop in temperature up to 15 K, in particular TK1-
1, TK 1, PYRO 3 and TK 3 are shown in Fig. 6, including 2. Maintaining a given temperature set point outside of the
their averages per step. It is immediately clear that control- furnace (PY1-n and TK1-n) does not guarantee a stable temper-
ling the furnace temperature via PYRO 3 is feasible: the set ature inside the furnace. This can be explained by the indirect
point tracking is adequate and the oscillations are limited for heating of the reactor outlet by the process gas causing the
all measurements, indicating stable operation. In step 4, the outlet temperature to respond slower to changes in the sys-
TK 3 temperature measurement is used to control the furnace tem, or by the fact that external influences, such as heat losses
while in steps 5–7, the PYRO 3 measurement is used. There is a due to convection, affect the temperature measurement out-
clear difference in time scales during step 4: when starting the side of the furnace to a greater extent than inside the furnace.
cracking experiment, the temperatures measured inside the The temperature in step 6 should increase by 10 K as com-
furnace (PYRO 3 and TK 3) reach steady state within minutes pared to the temperature in step 5. The temperature rise is
while the temperatures measured outside the furnace (PYRO 1 observed in all experiments and is consistent for the PY3-n
and TK 1) take around one hour to reach a steady state. Inside experiments but shows more erratic behavior for PY1-n and
the furnace, the reactor tube is directly exposed to the heat TK1-n. The temperature in step 7 should be 25 K above the
source and hence changes temperature quickly. The section temperature in step 5, which is again attained in PY3-n only.
of the reactor outside of the furnace, where TK 1 and PYRO 1 Even though the difference in absolute temperature between
are located is heated indirectly via heat exchange from the hot PY3-1 and PY3-2 is around 6 K in step 7 as a consequence of
process gas to the process tubes. Due to this indirect heating, the choice of the temperature set point in step 5 where this
the response to a set point change was much slower for the difference was introduced. Temperatures for TK1-n and PY1-
temperature measurements outside the furnace as compared 2 end up significantly higher than the temperature in PY3-n.
to the temperature measurements inside the furnace. This This indicates how much the choice of the measured value for
also explains why the PYRO 3 temperature measurements are the temperature control loop influences the steady-state and
more sensitive to changes in process conditions compared to transient behavior of single measurement values such as the
TK 1 and PYRO 1 where there is more delay due to the indirect coil outlet temperature and by extension also the behavior of
heating by the process gas. the complete furnace. This wide spread on a primary process
A more rigorous analysis of the gathered data is required variable such as the coil outlet temperature should be kept in
in order to draw quantitative conclusions. In a first step, the mind when observing secondary process variables such as the
averaged process gas outlet temperature measured using TK 3 coil outlet composition or the amount of coke deposited.
per experimental phase as discussed in Section 2.4 is given in To further analyze this variation in the process variables
Fig. 7. Only the instantaneous measurement of the process gas and its dependence on the temperature measurement used for
temperature at the moment of injecting a process gas sample control, Fig. 8a shows the parity plots of the measured temper-
on the GC for analysis are considered. ature at certain axial positions in the final pass of the reactor
During step 4, the temperature in the furnace is con- coil against the temperature at those axial positions averaged
trolled via the default control system based on the process over all experiments.
gas measurement TK3. As the process gas temperature is A larger spread in the parity plot around the first diago-
the controlled variable during step 4, the measured process nal indicates a more erratic behavior at that point during the
gas temperatures are grouped closely together around the set experiments. The parity plot for temperature in Fig. 8a con-
point value of 1093 K, independent of the experiment. In the firms the observations made based on Fig. 7: PY3-n succeeds in
subsequent phases, the spread on the process gas outlet tem- controlling the temperature relatively well given the relatively
perature increases as different control systems are used. In small spread. The spread is higher for PY1-n and TK1-n as
step 5, the process gas temperature should maintain the same compared to PY3-n. Only a small number of the temperatures
Chemical Engineering Research and Design 1 5 3 ( 2 0 2 0 ) 380–390 387
Fig. 8 – Parity plots for temperature (a) and pressure (b) for the different experiments; Averages are taken for different axial
positions along the last pass of the reactor coil, over all experiments. The larger the spread in the parity plot, the more
erratic the control system behaved during the experiment.
Fig. 9 – (a) Ethane and (b) ethene weight percent at the reactor outlet for the different experiments, per step as described in
Section 2.4.
Fig. 10 – Amount of coke burned as a function of decoking Fig. 11 – Number of temperature measurement readings
time for the different experiments; inlay: rate of coke above a given arbitrary temperature threshold during
burned as a function of decoking time for the different cracking (steps 5–7).
experiments.
(Dente et al., 2007). Longer decoking times as a consequence coke which can easily be gasified, is removed. Towards the end
of a higher coke density and lower porosity is indicative of of the decoking process, the harder, denser coke is burned at
higher temperatures during the coke formation. Therefore, the a rate that is at least one order of magnitude lower compared
decoking time can be correlated to the temperature control to the beginning of decoking. In PY1-2, the total amount of
mechanism during cracking, in addition to the obvious link coke is the highest due to a higher deposit of porous coke
between the amount of coke deposited and the decoking time. which is easily burned off. In TK1-2, the total amount of coke
The average amount of coke deposited during the PY3- is also high but in this case, more dense coke is formed, as
n experiments is lower compared to PY1-n and TK1-n as seen from the long time until complete decoking. This can be
seen in in Table 1. Since during the PY3-n experiments, the explained by the occurrence of temperature peaks that caused
temperature in the last cell was directly controlled by a mea- rapid graphitization of the coke already present on the reactor
sured temperature in that cell, the number of temperature surface. In other words, one expects a correlation between the
overshoots that cause excessive coking could be minimized. number of temperature overshoots above a certain threshold
However, the average amount of time required to burn off a value on one hand and the amount of coke formed on the other
gram of coke is unexpectedly high for PY3-2. The amount of hand, which is confirmed by an a posteriori statistical analysis
coke formed was the lowest for all experiments but the time of all temperature measurements during the experiment, see
required to burn it off was high, pointing to denser coke. This Fig. 11.
is counterintuitive as the coke formed in the PY3-n experi- PY1-2 and TK1-2, the experiments with the highest amount
ments should be the most porous and hence the most easily of coke formed and the longest decoking time, also exhibit
removed, due to the absence of temperature overshoots. The the highest number of thermocouple measurement points
longest decoking time is observed for the PY1-2 and TK1-2 above a certain measurement value. Especially for tempera-
experiments, mostly because the amount of coke formed dur- tures beyond 1180 K, the correlation between the amount of
ing these experiments was the highest. However, the majority data points and the amount of coke formed is strong. It is strik-
of that coke was assumed similar in structure to the coke ing that TK1-1 has a high number of measurement points for
formed during the other experiments as the rate of coke burn- temperatures up to 1150 K. This did not influence the amount
off is nearly the same for all experiments, see the inlay in of coke formed significantly but it has an effect on the conver-
Fig. 10. In the beginning of the decoking process, the porous sion and the ethene selectivity as observed in Fig. 9.
Chemical Engineering Research and Design 1 5 3 ( 2 0 2 0 ) 380–390 389
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