Automation

Measuring
Engineering
Services
Process
Control
Control of
Low-Pressure
Carburizing
Processes
H. Altena
1
, F. Schrank
1
. S. Heineck
2
1
Aichelin Ges.m.b.H. Mdling, Austria
2
Stange Elektronik GmbH. Apfelstdt, Germay







page 2 of 11

www.stange-elektronik.de
Control of low-pressure carburizing processes

H. Altena
1
, F. Schrank
1
. S. Heineck
2
1
Aichelin Ges.m.b.H. Mdling, Austria
2
Stange Elektronik GmbH. Apfelstdt, Germay



Present low-pressure carburizing is controlled by computer optimized treatment programs. Up to now no
carburizing process in-situ control was possible. This restricts process monitoring and quality control.
Insufficient carburizing by non-optimized gassing or too low gas amounts could not be recognized or
corrected during the process.

The development of a low-pressure carburizing sensor that determines the degree of reaction of
acetylene by measurement of H
2
concentration in the furnace hot zone is reported. It is shown that the H
2
concentration depends significantly on batch surface area, loading density, treatment temperature and
gas flow rate. The developed correlations permit low-pressure carburizing process monitoring as well as
process control.

For the first time for low-pressure carburizing an in-situ monitoring of the pyrolysis reaction is possible by
the introduction of a low-pressure sensor. This represents substantial progress in quality control of low-
pressure processes. Furthermore through H
2
measurement results can be controlled from the reaction at
the component surface, also carburizing problems can be recognized and/or avoid by process control.

The results of this comprehensive study are presented and the actual state of development discussed.


1. Introduction

Since ISO 9000 implementation quality awareness and quality control became more important and are
now essential in all fields of heat treatment. Compliance within narrow tolerances throughout the whole
production process, beginning with material composition up to heat treatment, is required for modern
production processes. For case hardening the following customer requirements must be fulfilled:

- Narrow heat treatment tolerances
(Surface C, C profile, case depth, core strength)
- Reproducibility of treatment result
- Low surface layer mechanical damage
- Low heat treatment distortion
- Process control and documentation
- Low heat treatment costs

Low-pressure carburizing processes can fulfil a lot of these requirements and became an alternative
solution to conventional gas carburizing over the past years.
The "vacuum carburizing" disadvantages in the 150 - 600 mbar pressure range was overcome by
carburizing in the mbar range as well as changed system technology [1]. While the new technology was
used rather quickly in France, it was often touched with scepticism in German-speaking countries.







page 3 of 11
This scepticism principally consists of:

- memories of negative experiences with process engineering problems using older "vacuum
carburizing", like soot formation in the furnace and low loading density as well,

- failed attempts for control of the carburizing process. High demands on quality control and
process control were contrary to low-pressure carburizing distribution in start-up period.

Low-pressure carburizing processes are currently controlled by preset, computer optimized treatment
recipes [1-3]. This is a kind of restriction for process monitoring, because no in-situ control is possible.
According to this, insufficient carburizing due to incorrect gas flow rates can not be either recognized as
well corrected during the process.


2. Control of low-pressure carburizing processes

During low-pressure carburizing the C-
transition occurs by pyrolysis reaction of the
carbon carriers (mostly propane or
acetylene) at the hot component surface. No
balance reaction occurs by the pyrolysis so
no c-level is definable which guides to a
carbon-balance-concentration in the work
piece that is already established from
atmosphere carburizing. (Figure 1).
Atmosphere
gas
carburizing
When low-pressure carburizing a very fast
rise of surface C-content to the absorption
limit happens. In order to improve the
uniformity of carburizing, the carburizing
process is interrupted after a few minutes
and a diffusion phase is attached, where the
process gas is evacuated from the furnace
and carbon diffuses into the base material
[2,3]. This interruption is followed by a new
carburizing cycle (Figure 2)

www.stange-elektronik.de
Figure 1: Equilibrium condition and C oversaturation at
atmosphere gas carburizing gas and LP-carburizing
(according to D. Grassl)




Figure 3:
Low pressure carburizing / Process
diagram (schematic)




















page 4 of 11
To avoid over-carburizing and strong carbide formation, usually a reduced gas flow rate will be used.
Alternatively the proportion of carburizing to diffusion time can be reduced with constant gas amount.
Because the carbide formation is relatively slow the C-absorption of steel decreases in case of exceeding
the carbide limit.
At the end of the carburizing cycle a longer diffusion phase follows, where the surface-C of saturation
concentration is reduced to approximately 0.7 - 0.75 %. As is the case of diffusion over 930C even
possible carbides are dissolved. The diffusion also contributes to uniform carburizing throughout the
batch, so that a high uniformity and quality of the carburizing process can be ensured.
Carburizing and diffusion can be simulated by diffusion calculation software. With the offline program
optimal treatment conditions can be selected as well gas flow rates and/or carburizing times can be
determined.
Although this process control works very reliable, this method has a certain restriction for process
monitoring and quality control because it provides no in-situ control of the carburizing process.


3. Low-pressure carburizing sensor

The propane pyrolysis first occurs by formation of H
2
CH
4
C
2
H
6
C
2
H
4
C
2
H
2
as well as smaller quantities of
long-chain molecules (Figure 3). C
2
H
2
and C
2
H
4
react with the part surface, also the reaction catalyst, to
form H
2
and/or CH
4
and to carburize the part surface [1].
Also the acetylene pyrolysis of C
2
H
4
takes place over several intermediate products, but leads in sum to
diffusion of C with formation of H
2
and small quantities of CH
4
.


Figure 3: Pyrolysis of propane and acetylene

By measuring of the exhaust gas the concentrations of the reaction products - i.e. predominantly H
2
, CH
4

as well the sum of C
2
H
x
molecules - were determined (Figure 4). It could be shown, that the propane
pyrolysis is significantly faster than the pyrolysis of acetylene. Within 3 minutes a constant gas
composition from 54 - 55 % H
2
and 25 % CH
4
was acquired. With acetylene gassing at 930C an H
2

concentration of approx. 35 % was determined, which increased further with longer treatment times or
higher temperatures by pyrolysis of remaining C
2
H
x
molecules [3].
So it seemed to be purposeful to monitor the carburizing reaction by measurement of the H
2

concentration. Furthermore it was expected that propane pyrolysis would yeild an in-situ H
2
-concentration
measurement that would represent the reaction process and enable process control also.

www.stange-elektronik.de







page 5 of 11


Figure 4: Low-pressure carburizing with high pressure gas quench (exhaust gas analysis)

Hydrogen sensors are already successfully used for monitoring and control of nitriding process, for which
the H
2
-measurement takes place at atmospheric pressure. An existing sensor must be adapted in such
way that it can be used in vacuum. The decision was made to use the Stange Elektronik H
2
sensor, which
determines the H
2
concentration based on a heat conductivity measurement principle and fulfils following
requirements:

- Low dead time
- High response sensitivity
- No cross sensitivity e.g. compared to CH4 and other process gases
- No pressure dependence of measurement signal
- Vacuum solid

The sensor had to be adjusted to the specific requirements, where especially high response sensitivity in
the mbar range as well as a sufficient accuracy of measurement was the greatest challenge.


3.1. H
2
sensor mode of operation

The measuring principle is based on the fact that hydrogens heat conductivity is much greater than those
of all other gases (Figure 5).



Figure 5: Relative heat conductivity of gases compared with air (at 100C) (Documentation of Hartmann & Braun AG,
Frankfurt)

www.stange-elektronik.de







page 6 of 11
The device is based on a Wheatstone bridge which consists of four measuring curvettes. Two parallel
curvettes are located in the gas flow. The other two are surrounded by a reference gas. The produced
electric signal is a measurement for the hydrogen concentration of the analysed gas (Figure 6).


Figure 6: Measuring principle (H
2
-Sensor)

It is essential that the measuring cell is surrounded by a measuring gas according to the hydrogen
diffusion principle and achieves a temperature which depends on the heat conductivity of the measuring
gas. The bridge connected curvettes are characterized, that the measuring cells are non-catalytic and the
heats of reaction are measured. An external pressure sensor is used for compensation of the H
2
sensor
measurement signal. The different reaction times of the signals were to be considered.
The sensor was connected to a flange located in a water-cooled double jacket (Figure 7).


Figure 7: Measurement setup (H
2
-Sensor)

www.stange-elektronik.de







page 7 of 11
4. Required gassing quantities

Due to the high carbon availability the rise of surface C-content up to saturation happens within a few
minutes during low-pressure carburizing processes. The ideal C mass flow rate which is needed for
maintaining the saturation concentration decreases with preceding treatment duration (Figure 8) based on
the t-law.


Gas flow rate m
c
[g/m
2
h]

Figure 8: C evacuation by diffusion (C = C
5
)

The intent of H
2
sensor carburizing control is to set the gas flow rates by H
2
measurement signal. So that
inequalities in carburizing can be prevented and on the other hand over-carburizing and/or carbide
formation will be prevented.
This should be possible at constant pulse-pause ratio with decreasing gas flow rates, as well as variable
pulse-pause ratio and largely constant gassing quantities.


5. Results of measurement

To achieve the desired sensor responsivity, the measurement setup had to be optimized as well the
measurement signal needed to be electrically amplified. The calibration of the measurement signal was
done with reference gases which were made by defined compositions. This optimization now permits an
in-situ measurement of the pyrolysis of propane and acetylene by measurement of H
2
concentration with
sufficient accuracy.
The analysis takes place in today's usual temperature range from approx. 860 - 1000C, whereby most of
the tests were made at 930 C. The batch surface areas were varied between 1 and 8 m
2
, the batch size
was approx. 600 X 600 X 600 mm (single batch). The gas flow rates were varied in test programs
according to requirements.


5.1 Gassing with propane

The Carburizing took place at 930 C; the proportion of gas flow rates to batch surface areas was varied
within one dimension. In Figure 9 the H
2
signal is compared at 1 and 4 m
2
. The H
2
content was in the first
cycle approx. 54 % and increased with further gassing up to 55 %. The build-up of sensor signal took
place faster naturally at greater gas flow rates (900 I/h).


www.stange-elektronik.de







page 8 of 11

Batch surface area
Gas cycle
Figure 9: H
2
measuring values with propane gassing (influence of batch surface)

The H
2
concentrations of the in-situ measurement were the same value as the exhaust gas
measurement, which was measured in earlier tests. Contrary to expectations the considerably different
batch surface areas (1 to 4 m
2
) resulted in a very small change of H
2
concentration or H
2
measurement
progress.

As well changes of gas flow rates did not lead to a clear change of the measurement signal. The results
of these tests were very reproducible. Also after improvement of the sensor sensitivity no significant
influence of gas fow rates and batch surface areas on measurement signal could be realized. Because
the measurement signal gave no conclusions to batch carbon requirements and the process gas carbon
effect, it seems not to be suited for in-situ measurement or control.


5.2. Gassing with acetylene

Acetylene gassing takes place at first analogue to propane test at 930 C with 1 and/or 4 m
2
batch
surface areas and variable gas flow rates. The H
2
measurement now shows a clear batch surface
dependency (Figure 10). The first cycle leads to a very high crack level at 4 m
2
batch surface area
regardless of a relatively huge amount of gas, which refers to a lack of process gas. On the other hand at
1 m
2
surface the crack level was just under 50 % in the first cycle.


Batch surface area
Gas cycle
Figure 10: H
2
measurement values at acetylene gassing (influence of batch surface)

www.stange-elektronik.de







page 9 of 11

Changed carburizing temperatures of 860 C as well as 1000 C result in slightly different H
2
measuring
values as expected, which document the temperature dependency of acetylene pyrolysis as well as
carbon absorption of the steel. The batch surface area was enlarged up to 8 m
2
in these tests. A rise of
the H
2
measurement signal was noticed with increasing treatment temperatures. In order to implement
the H
2
concentration as a measurement signal for the process control, a correlation between crack level
and a satisfying carburizing cycle must be made, where no inequalities at carbon absorption or over-
carburizing and carbide formation occur.
Low-pressure carburizing processes are relatively "good-natured", regarding the required gas flow rates
in dependence of the batch surface [3]. With acetylene an under-run of the "minimal gassing" does not
lead to serious inequalities of carburizing, like in case of propane. In result of this there should be a
relatively wide range, where a satisfying carburizing cycle can be done.


Figure 11: Range of optimal H
2
concentration with acetylene gassing

In scope of the extensive tests, the range was determined with respect to the treatment temperature
(Figure 11). A largely linear dependence of an "optimal" H
2
concentration from treatment temperature
follows.


5.3 Reproducibility

A pre-cursor to use a measurement signal for control purposes is a sufficient reproducibility of the
measurement signal. It could be verified, that repeat of the tests with identical conditions lead to very
good reproducible H
2
signals; the maximum deviation amount was 2%. Furthermore it was detected that
the measurement signal showed no drift over a period of several months.

www.stange-elektronik.de







page 10 of 11
6 Process control

The target values of temperature-dependent and optimal H
2
concentration makes a process control by
adjustment of the acetylene gassing rate possible (Figure 12). In the case of process control with
constant carburizing-diffusion cycles, the gas flow rate is based on C-absorption of the material to
constant H
2
concentration can be controlled within the "process window" (Figure 11). The gassing here is
adapted to the decreased carbon absorption of the treatment material.


Figure 12: Control loop for low-pressure carburizing processes (diagram)

Alternatively the carburizing can be done with increasing diffusion durations between the individual
gassing cycles. The duration of carburizing and diffusion times is calculated with FOCOS Simulation
Calculation software.
The program should result in a rise of surface-C-content to each 1,3 % with a decrease to 0,8 % during
the diffusion phase. The advantage of this process control is that over-carburizing and carbide formation
can be avoided easier. A disadvantage is the 20% to 30 % extended process time (carburizing and
diffusion phase).

Even with such a kind of changed process management, the process control by H
2
concentration
measurement appears reasonable, because the gassing quantity is set with respect to the batch surface
area.
Contrary to the described carburizing process, the gas amount during the carbon cycles stays largely
constant with correct calculation of the diffusion time.


7. Conclusions and forecast

The compliance of close tolerances and reproducible heat treatment quality are necessary requirements
for modern heat treatment systems and processes. In-situ measurement and carburizing control with
oxygen sensors allows the fulfilment of these requirements for atmospheric carburizing processes.
However, low-pressure carburizing is currently controlled according to given, computer-optimized
treatment programs.
A low-pressure carburizing sensor was developed, which determines the performance grade of the
acetylene pyrolysis by measurement of the H
2
concentration in a furnace hot zone. It was shown that the
pyrolysis depends largely on batch surface areas, gas flow rates and treatment temperatures. In result
the H
2
measurement can be used for process monitoring and control.

www.stange-elektronik.de







page 11 of 11

www.stange-elektronik.de
Compared to that, propane pyrolysis takes place much faster and leads to a result of constant H
2

concentration. This shows no significant dependence of process parameters and currently allows no
control possibility using the H
2
sensor.

The introduced low-pressure sensor makes an in-situ measurement and process control of acetylene
carburizing possible for the first time. This represents an important improvement for low pressure
carburizing processes.
A changed measurement setup as well an increased H
2
measurement accuracy could be the
requirements for process control with propane gas. Even here, corresponding approaches show
development possibilities.


8. Literature

[I] Altena, H.: HTM 49 (1994) 1, S. 58 63.
[2] Lser, K.: Tagungsband der Europ.Tagung; Das Einsatzhrten", Zrich, CH, 3.-4.4.2003; S. 115 122.
[3] Altena, H.; Schrank, F.: HTM 53 (1998) 2, S. 93 101.
[4] Altena, H.; Schrank, F., Heineck, S.: HTM 61 (2006) 4, S. 195 206.