Sulphur content estimation of Venezuelan

heavy oil by fast neutron and gamma

transmission technique

F. Pino, L. Stevanato, D. Fabris,

H. Barros, A. Vidal, G. Nebbia,
M. Lunardon, S. Moretto & L. Sajo-
Bohus
Journal of Radioanalytical and
Nuclear Chemistry
An International Journal Dealing with
All Aspects and Applications of Nuclear
Chemistry

ISSN 0236-5731
Volume 314
Number 3

J Radioanal Nucl Chem (2017)

314:1833-1839
DOI 10.1007/s10967-017-5533-2

1 23
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J Radioanal Nucl Chem (2017) 314:1833–1839
https://doi.org/10.1007/s10967-017-5533-2
Sulphur content estimation of Venezuelan heavy oil by fast
neutron and gamma transmission technique
F. Pino1,2 • L. Stevanato2 • D. Fabris3 • H. Barros1 • A. Vidal1 • G. Nebbia3
M. Lunardon2 • S. Moretto2 • L. Sajo-Bohus1,2
Received: 31 July 2017 / Published online: 10 October 2017
Ó Akadémiai Kiadó, Budapest, Hungary 2017
Abstract A compact and modern equipment for imple-
menting the fast neutron and c-ray transmission technique
(FNGT) has been developed in order to estimate the sul-
phur content of crude oil. FNGT is employed for non-
destructive analysis of different kinds of samples. The
compact system presented in this work represents an
improvement of our previous experimental set-up [1, 2]. It
makes use of a 252Cf source, an EJ-301 liquid scintillator
detector (200 9 200 ) with excellent n/c discrimination
capabilities, and modern nuclear electronics based on fast
digitizers. The fast neutron and gamma transmission
technique was employed to study a system for on-line
sulphur concentration measurement in Venezuelan heavy
sour oil. The range of sulphur concentrations investigated
is between 0.1 and 6.5 wt%. The equipment performances
and limitations are compared with those predicted by a
Monte Carlo model built in GEANT4 v10.01. The results
show the possibility to implement a compact unit for on-
line determination of sulphur concentration in crude oil.
Keywords Fast neutron and gamma transmission 
Sulphur content  Heavy-sour oil  Monte Carlo simulations
& F. Pino
felixpino@gmail.com
1
Universidad Simon Bolivar, Ap.do 89000, Caracas 1080A,
Venezuela
2
Dipartimento di Fisica ed Astronomia dell’, Università di
Padova, 35131 Padua, Italy
3
INFN Sezione di Padova, Via Marzolo 8, 35131 Padua, Italy
•
Introduction
Non-destructive analysis of materials that make use of
techniques hinging on fast neutron and c-ray transmission
have been studied in the past in different landscapes [3–6].
X-ray scanners are widely used in homeland security
applications and they produce high resolution images. In
addition, photon inspections provide material recognition
when special technologies such as ‘‘dual energy radiog-
raphy’’, ‘‘backscatter imaging’’, etc. are implemented [3].
The use of fast neutrons as probing radiation and even the
combination of those and c-rays has been often proposed in
the past. Its design required sophisticated techniques to
provide an improved material recognition, especially for
materials with a low mass value and low atomic number.
The objective of introducing neutrons was to optimize the
detection capability for hidden explosives and drugs in
customs operation in which C, O and H nuclei are major
components. Examples of such developments are the
‘‘combined fast-neutron with gamma-radiography’’ and the
‘‘fast neutron resonance radiography’’ techniques [4–6].
Most of the experiments have been conducted using neu-
tron/gamma sources having very complex arrangements
based on nuclear reactions produced by accelerators, for
example employing as a neutron source d(d,3He)n and
9
Be(d,n) reactions. In order to reduce the experimental
complexity, Viesti et al. [1, 2] implemented the ‘‘fast
neutron and gamma transmission’’ (FNGT) technique using
a fission neutron source of 252Cf; the experiment results
were a highly successful advancement in material recog-
nition. The experimental systems were based on the time of
flight technique in order to discriminate between neutrons
and c-rays. The drawbacks of this technique are the
necessity of very long measurement time and/or a very
intense neutron source.
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The reported non-destructive technique with neutrons
and c-rays has been often implemented in industrial envi-
ronments. The most popular is the on-line implementation of
the FNGT technique required to control coke moisture [7, 8]
(a parameter of particular importance in steel manufactur-
ing). Some applications initiated by Viesti et al. [1, 2] are
studied in details, including the use of FNGT for monitoring
the sulphur content in crude oil. In relation to the sulphur
content, problem also found in the coal industry, other
nuclear techniques, as prompt gamma neutron activation
[9, 10], have been proposed and applied. The alternative
technique suggested by Viesti et al. [1] has several advan-
tages concerning industrial applications; in fact, it was
demonstrated that the FNGT technique has a very good
resolving power to determine the average atomic number of
compounds with low atomic number (Z \ 13). In this range
of values lay also the crude oil elemental composition,
therefore we suggest to employ the mentioned technique for
monitoring sulphur content in the oil industry.
There are many reasons why it is of importance knowing
the sulphur content of crude oil. Sulphur concentration may
vary by a factor of ten depending on the exploitation site
[11]. A widely used scheme for classifying crude oils is
based on their API gravity (specific gravity) and sulphur
content. Each crude class is defined by a range of API gravity
and a range of sulphur content; the names of the categories
indicate these ranges in qualitative terms [12, 13]. For
example, ‘‘light sweet’’ crude oil has a specific gravity
between 35 and 60o API and a sulphur content between 0 and
0.5 wt%, while, ‘‘heavy sour’’ crude oil has a specific gravity
between 10 and 26o API and a sulphur content between
greater than 1.1 wt%. The Venezuelan crude oil produced in
the so-called Orinoco Oil Belt, part of a larger subsoil
reserve called East Venezuelan Basin (see Fig. 1), is of the
heavy-sour type having values of API gravity between 4°
and 17° and sulphur content between 3 and 4 wt%.
Fig. 1 Schematic map of the
Venezuelan crude oil field
called ‘‘The Orinoco Oil Belt’’
representing Machete, Zuata,
Hamaca and Cerro Negro
exploitation sites that is part of
reserve region included in the
East Venezuelan Basin
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J Radioanal Nucl Chem (2017) 314:1833–1839
The API gravity and sulphur content of the crude oil, are
related by a typical exponential function given in Fig. 2.
Crude heavy oil often is rich in hetero-elements but
sulphur has the most devastating effects on the refinery
piping system [14–16]. Even in relatively low concentra-
tion in refinery streams sulphur can (a) deactivate (poison)
the catalysts that promote desired chemical reactions in
certain refining processes, (b) cause corrosion in refinery
equipment, and (c) lead to emissions of sulphur compounds
in the atmosphere. The latter is quite undesirable and
subject to stringent regulations. In long transferring
pipelines sulphide scales represents the main deterioration
on the steel surface [15]; its effect is related to changes of
steel micro-structure and to the production of internal
corrosion with the consequence of metal release often
being the cause of high economical losses. Consequently,
refineries must have the capability to remove sulphur from
crude oil and refinery streams to the extent needed to
mitigate these unwanted effects.
Our aim is to develop a non-destructive analyzer (NDA)
based on a nuclear technique to provide sulphur concen-
tration values in real-time for crude oil. Nowadays, the
used technique requires several days in order to obtain the
information due the off-line chemical or nuclear analysis
[17, 18]. The refinery complex can take advantage of a
real-time measurement because the plant procedures can be
adjusted before oil arrival.
Theory
Material recognition can be obtained from Rn,c-ratio
[1, 2, 19, 20] based on absorption coefficients for fast
neutrons ln, and c-rays lc, or the logarithmic ratio of the
measured transmission factors for neutrons (In/In,0) and
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J Radioanal Nucl Chem (2017) 314:1833–1839
Fig. 2 Illustration of the typical behaviour between the API gravity
value and the sulphur content in Venezuelan crude oil
gamma rays (Ic/Ic,0), respectively. Therefore, the following
relationship hold:


ln ln In In;0
Rn;c ¼ ¼   ð1Þ
lc ln Ic
Ic;0
where In and Ic (In,0 and Ic,0) are measured yields for
neutrons and c-rays with (without) the sample. The most
important outcome is that the Rn,c-ratio characterizes a
selected sample independent of its thickness or geometrical
shape; the assumption is valid since multiple scattering
inside the sample has a negligible effect as was confirmed
experimentally by Viesti et al. [1].
Experimental
The early experimental set-up has been modified resulting
in a compact and highly reliable system made of a 252Cf
neutron source, a single liquid scintillator detector EJ-301,
with a good response for both fast neutrons and c-rays, and
a modern nuclear electronic setup based on fast digitizers
(for digital processing of the signals). A Monte Carlo
model based on the GEANT4 v10.01 code was built in
order to optimize and evaluate the response and the effi-
ciency of the system. A schematic lay-out of the experi-
mental set-up is given in Fig. 3.
The sample and radioisotope source holder are posi-
tioned at 30 cm from the front-face of the scintillator
detector coupled to the electronic chain. The detector is of
a cylindrical EJ-301 liquid scintillator cell of 5 cm in
diameter and 5 cm thickness, coupled to an H1949-51
HAMAMATSU linearly focused 12 dynodes photomulti-
plier (PMT) through an EJ-560 silicone optical interface.
The operating voltage was set at - 1500 V. The front-end
electronics used in this work was composed of the
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Fig. 3 Schematic representation of the experimental setup employed
for the measurement
following CAEN VME modules: a V6533 Programmable
HV Power Supply (6 Ch., 4 kV, 3 mA, 9 W), a V1730
Digitizer (14 bits, 500 MS/s), and a Bridge USB V1718
connected to a PC with a data acquisition software. Inside
the digitizer, Digital Pulse Processing (DPP) algorithms are
implemented using a FPGA, providing pulse on-line anal-
ysis for each event obtaining: (a) timestamp, (b) complete
integration of the signal, (c) partial integration of the signal
used for Pulse Shape Discrimination analysis and (d) the
possibility of storing a selected part of the digitized signal.
The optimization of the DPP parameters was obtained as
described in [21]. A 105 fissions/s 252Cf source was used.
Mono-elemental samples (with thickness from 1 to
3 cm) were used to calibrate the system as reported by
Viesti et al. [1]. A second group of compounds was used to
simulate the composition of the crude oil with different
sulphur contents (from 0 to 6 wt%). The sample is made of
a plastic cylindrical container filled by common engine oil
(with a negligible sulphur content), and a sulphur disk of
known mass attached on the top. An appropriate Monte
Carlo simulation was carried out to demonstrate the neg-
ligible effect in using two compound’s layer instead of a
homogenously mixed sample.
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Neutron and gamma transmission modelling
Monte Carlo simulations provides an important tool in
the design of nuclear detection systems and it is therefore
interesting to assess the capability of such calculation by
benchmarking with experimental results. In this work a
GEANT4 v10.01 toolkit [22, 23] was used to perform
Monte Carlo simulations of the sample geometry in order
to compare the measured neutron and gamma transmis-
sions with the simulated results, and to better understand
the system physical response and limitations.
Once the neutron interacts with the scintillator mate-
rial, several charged particles (recoil protons and carbon
ions) are produced; depending on their energy and
position they may either fully deposit their energy or
undertake partial energy deposition and leave the scin-
tillator sensitive volume. The light produced through the
interaction of these charged particles is related to their
kinetic energy via an appropriate light output formula
[24]. GEANT4 offers access to particle tracking (posi-
tion/time of the particle, kinetic energy, deposited
energy, etc.), by means of its G4Track.hh yielding the
kinetic energy of the recoil protons and carbon ions. In
case of simulations of photons, GEANT4 standard phy-
sics libraries reconstruct all important interactions in the
energy range of interest (e.g. Rayleigh scattering,
Compton scattering, photoelectric effect and electron–
positron pair production).
The geometrical model considered was similar to the
actual experimental set up. All the samples, i.e. mono-
elemental and multi-elemental compounds were simulated
with the geometry employed in the experiments. A second
group of samples, i.e. crude oil, were also simulated taking
care of reproducing laboratory geometry, but using a single
compound with different quantities of H (10–14 wt%), C
(83–85 wt%), N (0.05–2 wt%), O (0.05–1.5 wt%) and S
(0.05–6 wt%) equally distributed. The gamma and neutron
spectra of the 252Cf were simulated accurately, using the
Watt distribution for neutrons, while the gamma energy
spectrum was taken from experimental data available in the
literature [25]. Each run consisted of 4 9 107 neutrons and
108 gammas being carried out separately (initial direction
of the particles was toward the sample).
Results and discussion
The analysis was performed using ROOT software [26]. An
example of the outcome for a blank 252Cf is illustrated in
Fig. 4.
Neutron and gamma related pulses are reported in a PSD
parameter-light output diagram (two-dimensional spec-
trum). The best gate setting was obtained following
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Fig. 4 Two-dimensional spectrum showing the neutron/gamma dis-
crimination. The c-ray events are found in the lower branch and the
neutrons are depicted above the boundary line. Colors are related to
the count rate and are indicated for reference. (Color figure online)
Stevanato et al. (FoM) [21]. Energy calibration of the
detector was made from 22Na spectra following the method
reported by Stevanato et al. [27]. The continuous line
between the two regions shows the boundary line sepa-
rating neutrons from gamma events. It was defined by
doing the same analysis with a pure gamma source (i.e.
22
Na). The results show that the PSD parameter provides a
good separation of gammas from neutrons; the method is
an alternative to that obtainable by TOF-technique that
requires almost 1 m of time of flight and a dedicated
detector for triggering the fission events. The compactness
of the assembly ensures a higher counting efficiency thus
requiring shorter acquisition time to get significant statis-
tics. Each measurement performed in this work was
obtained in a time interval of 15 min (time of flight tech-
nique requires around 6 h of acquisition time to get
equivalent statistics). In the R value calculation, the same
threshold on light output was used both for laboratory
measurements and Monte Carlo simulations. The value was
set at 50 keVee.
The mono-elemental and mixtures samples R values are
obtained as a function of their effective atomic number and
it is shown in Fig. 5.
The measured data provide an average calibration line
(R vs. Z). Monte Carlo results are also reported for com-
parison in Fig. 5. It can be seen that there is a remarkably
good correspondence between the experimental and simu-
lated results. The fit (power equation) was applied to the
experimental results obtaining similar fitting parameters as
reported by Viesti et al. [1]. It should be noted that the
mentioned results are very similar but in our case the
measurements time interval was reduced by a factor of 12.
And also, due to the fact that in this case we have used a
smaller detector, a different arrangement of the
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J Radioanal Nucl Chem (2017) 314:1833–1839
Fig. 5 The measured values of Rn,c are given as a function of sample
effective atomic number for a large set of pure elements and
compounds. Experimental uncertainties are 2.2% (see Fig. 6).
Uncertainties of the simulated results are smaller than the size of
the marker
Fig. 6 Histogram of the frequency for a set of 25 Rn,c-values of the
same sample
experimental set-up parts and a different approach to per-
form the analysis of the measurements (in particular the n/c
discrimination), these results demonstrate that the calibra-
tion curve does not depend on geometry.
In order to establish the reproducibility of the analytical
system and a reliable uncertainty of the Rn,c-values, one
sample (choose randomly) was used to perform several
measurements during 24 h (without altering the geometry,
15 min each run) obtaining a set of Rn,c-values which are
shown in Fig. 6. A histogram was superimposed to deter-
mine the technique precision.
The standard deviation of the distribution was found to
be 2.2%. This value is in excellent agreement with the
value determined by applying error propagation theory
over Eq. (1), taking the uncertainties of the neutron and
gamma intensities (In, In,0, Ic and Ic,0) as the root square of
1837
the number of counts (Poisson statistics). From now on,
2.2% will be the associated uncertainty of the experimental
Rn,c-values in this work. It is interesting to stress that if one
wants to reduce the uncertainty to 1%, the fission rate of
the 252Cf source should be increased by one order of
magnitude (i.e. 106 fissions/seconds).
In Fig. 7 the experimental and Monte Carlo simulation
results of the Rn,c-values associated to the crude oil sam-
ples with different sulphur concentrations are shown. The
experimental Rn,c-values are well represented by a com-
pound with an effective atomic number around Zeff * 3,
which is very close to the Zeff of crude oil (calculated
according to its well-known major composition). Over
1.5 wt% of sulphur content, a linear trend of the data is
observed. An also, according to the parameters of the linear
fits (Rn,c = B ? A  Cs), a very good agreement between
the experimental and simulation results is found.
The Monte Carlo results indicate that the determination
of the sulphur content for concentrations lower than
1.5 wt% suffers high uncertainty, however, it is much
better for the sulphur concentrations region corresponding
to heavy-sour crude oil, where the technique is intended to
be used.
In order to have an idea of the accuracy of the mea-
surements, taking as a reference the Monte Carlo results,
the inset in Fig. 7 shows the residuals, that is the differ-
ences between the Monte Carlo linear fit and the experi-
mental values. As can be seen, the residuals are lower than
2% for sulphur content greater than 1.5 wt%. From this
result, it can be said that the accuracy of the method is
acceptable. Concerning the precision of the technique,
from the ‘‘A’’ parameter of the experimental fit, we
obtained that for a Rn,c variation of around 2% (which is
close to the error bars in Fig. 7) there is a deviation of
around 1 wt% in the sulphur content. It should be stressed
that an easy way to improve the precision of the technique
is to increase the intensity of the neutron/gamma source.
Even if the precision of the results is very low, the
results given by this technique could be very helpful for the
oil industry. The possibility to have an on-line gauge which
gives even a rough information about the sulphur content
of the crude oil will be very favourable for the refining
process. Our technique is not intended to give a very high
precision results.
Taking advantage of the Monte Carlo simulations
capability, it was convenient to study the radiation buildup
effect on the Rn,c-values and on the overall sensitivity of
this technique. Since in the experimental set-up, the 252Cf
source is not collimated in a ‘‘narrow beam’’, it is possible
that the detector responds to both neutrons and c-rays
coming directly from the source or from scattered radia-
tion. It is really difficult to distinguish between these kinds
of events experimentally but, using the Monte Carlo model
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1838 J Radioanal Nucl Chem (2017) 314:1833–1839

Fig. 7 Rn,c-values as a function

of the sulphur content (wt%).
Uncertainties of the simulated
results are smaller than the size
of the marker

Conclusions

The results given in this work indicate the possibility to

Fig. 8 Experimental and simulated neutron spectra for the 5 wt% S
crude oil sample. The discontinuous line shows the buildup compo-
nent of the total spectrum
dealing with this quest, it is possible to know each com-
ponent of the spectrum. In Fig. 8 an example is given of the
experimental and simulated neutron spectra acquired by the
detector with one of the crude oil samples having a sulphur
content of 5% by weight.
As can be seen around 10% of the events are due to the
buildup effect. In the gamma spectra only 2% of the events
are buildup-events. If one makes the correction for these
events (by subtracting them from the total spectrum) the
Rn,c-values are slightly different from the original ones
(taking into account the total spectrum), however, the
sensitivity of the technique (slope of the fitted line in
Fig. 7) does not change significantly.
develop a compact and modern equipment for quality
control of heavy-sour oil (sulphur content greater than
1.5 wt%) with the aim to provide a new technical tool to
Venezuelan oil refineries. This non-destructive analysis to
estimate sulphur content has been demonstrated experi-
mentally and proven by Monte Carlo simulation. The
experimental results described in this paper show that this
method is fully adequate in the range of average Rn,c-value
corresponding to sulphur concentration of interest to the
Venezuelan crude oil refineries. The technique showed a
lack of accuracy in the region of sulphur concentration
below about 1.5 wt%, nevertheless for highest values of
sulphur content it offers a good accuracy and an accept-
able precision. However, higher precision could be
obtained increasing the source intensity within reasonable
bounds (and keeping the short time intervals for the anal-
ysis). The device operational range, as it is, is fully suit-
able to analyze Venezuelan oil type or extra heavy oil. In
particular, results show that this analytical technique copes
well with the industrial requirements to characterize on-
line crude quality well before being processed at the
chemical plant. A set of samples prepared in the laboratory
were measured in order to have a sufficiently developed
technique, the next step could be to provide a field-based
equipment to perform real tests in on-line monitoring of
crude oil sulphur content.

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Acknowledgements The co-authors F. Pino and L. Sajo Bohus are
indebted for the financial support as invited visitors to the University
of Padova.
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