1. Introduction
Gas leak detection is an important issue in production processes to prevent safety hazards and to ensure functionality of many products. For natural gas pipeline surveillance, many instrument developments aim at fast and sensitive remote detection of gas leaks. For these purposes gas cameras using modified thermal imaging systems, handheld tunable laser spectroscopy (TLS) instruments, and even helicopter-based systems are available [
1,
2,
3,
4,
5]. Commercially available handheld TLS instruments in the NIR are able to detect CH
4 leaks with column densities >1 ppm·m via remote detection. They can be used from a distance up to 30 m and have measurement rates up to 10 Hz [
3]. Determination of leak rates is difficult for remote gas detectors since sufficient information about the gas dispersion in the surrounding environment is usually not available. Recently, a TLS remote detection device was able to identify a CH
4 leak flux of 15 mL/min from a distance of 37 m [
6]. However, all these systems rely on infrared absorption of the target gas, which is the case for hydrocarbons, for example. Consequently, leak detection of non-infrared absorbing gases such as N
2, H
2, Ar, etc., is not possible in this fashion.
Sensitive leak testing of vessels, tubes, vacuum parts, refrigeration systems, etc., is usually performed via helium (He) leak testing. This detection method is based on a mass spectrometer (MS) that is tuned to He. In most cases, the examined object has to be filled with a He-containing gas. In such a leakage scenario, the He is detectable by pumping (“sniffing”) the leakage gas into the MS through a handheld nozzle located close to the leak. Very small leaks (below 10−7 mbar·L/s) can be detected by this method, but a close contact to the object is required. Apart from that, He leak testing from a distance is not possible. Further disadvantages are that the testing is a slow and manual task. A less expensive alternative to He is hydrogen or forming gas that is used in combination with sensitive electrochemical, metal oxide-, or Pd-based detectors. However, the use of hydrogen could be a safety hazard.
Acoustic leak detection is another common method. This method is based on the principle that the leakage gas generates a sound wave which can be detected by a sensitive microphone. Therefore, the object needs to be pressurizing in order to obtain a turbulent flow at the orifice which is required to generate (ultra-) sound waves [
7]. This may be circumvented by using an active ultrasound source within the object, but discrimination of the different sound paths could be difficult.
The classical leak detection technique for rather coarse leaks is the well-known “air bubble” method. A vessel under investigation is pressurized with gas (e.g., air) and immersed into a liquid (e.g., water). Air bubbles originating from the leak indicate the leak location and leak size. Minimum leak rates ≥10
−3 mbar·L/s can be detected by this method which is comparable to acoustic leak detection [
8]. Obviously, this method is not practical or feasible for large objects. Furthermore, the method is, generally, a slow and manual task. However, this concept may also be transferred in the gas phase. Therefore, a background gas in the atmosphere substitutes the liquid such that the background gas is displaced and diluted by the leakage gas. Thus, remote leak detection of any target gas—also of non-IR-active gases—should be feasible by a sensitive tunable laser spectroscopy (TLS) measurement of the background gas concentration. Ubiquitous and IR-active background gases are, for instance, CO
2, O
2, or H
2O, which should be different from the target gas. In order to detect a leak-induced ambient background concentration change, the distance has to be fixed or measured simultaneously [
9]. This can be achieved with state-of-the-art laser rangefinders.
In the next section, we show that O2 is the optimum candidate for a suitable background gas. Then the experimental setup is explained. Because of the visibility of the employed laser we use the term “LeakEye” for our technique. Computational fluid dynamics (CFD) simulations of the experimental setup are performed using COMSOL Multiphysics® (COMSOL Inc., Burlington, MA, USA). Then the results of experiments on extractive detection—later on, standoff detection—are given. In this work the terms non-tactile and standoff detection are synonymously used, even for rather short distances. The essential difference to extractive detection is that gas flow is not disturbed. We shall always compare experiments with direct (positive) detection of CH4 and with corresponding experiments on indirect (negative) detection of O2.
2. Modelling
The fundamental relation of absorption spectroscopy is given by the Beer-Lambert law:
where
I(υ) is the frequency-dependent transmitted intensity after passing a measurement cell with an optical path length
d,
c is the gas concentration, and
α(
υ) is the frequency-dependent gas specific absorption coefficient, which is given by the product of the temperature-dependent line strength
S(
T,υ
0) at the characteristic absorption frequency υ
0, and the pressure- and temperature-dependent line shape function
g(
p,
T,υ − υ
0).
As a rule of thumb we assume that a 1% reduction of the effective absorption length d by dilution of the background gas by the leakage gas has to be measured with a laser spectroscopic setup. In a typical situation an undisturbed extension of the leaking gas plume up to approximately 1 cm from the surface of the leaking object is assumed. For larger distances strong dilution by ambient air flow is expected. As a result the “LeakEye” technique is practically limited to standoff distances of approximately 1 m. For larger distances the relative measurement effect is too small.
Relevant atmospheric background gases, such as O
2, H
2O, and CO
2, with infrared absorption data are available in the HITRAN database [
10]. Suitable absorption lines of these gases for typical ambient concentrations,
T = 296 K and
p = 1013 mbar were selected and laser spectroscopic measurements were simulated using Mathcad (PTC, Unterschleißheim, Germany). For a total optical distance of 200 cm the transmission signal change for a 1% change of the optical distance was determined. For all gases distributed feedback (DFB) laser diodes in the near infrared (NIR) are available. In the simulation laser emission powers were set to 3 mW. Photodiodes with optimum detectivities with respect to noise equivalent powers (NEP) for the selected wavelength ranges were chosen as detectors. A maximum total transmission of 1% was assumed to account for the weak signal for standoff detection. The resulting power changes at the detector ΔP with respect to the relative power changes ΔP
rel are shown in
Table 1.
The measurement of O
2 at 761 nm was selected as the best choice (cf.
Table 1): although TLS-based hygrometers could serve as an established platform [
11], the expected ambient fluctuations for H
2O, as well as for CO
2, are too high. The first experiments with CO
2 show that the measurements are strongly affected by the exhaled air of people in the lab; this effect is much stronger for CO
2 than for O
2. Additionally, for CO
2 at 2004 nm the sensitivity is expected to be limited by detector noise. A further reason for the choice of O
2 with respect to for the measurement at 761 nm is that TLS of O
2 has become an established industrial measurement technique. For commercially-available process instrumentation, a precision of 10
−3 for O
2 concentration measurements is achieved [
12,
13], and laser radiation at 761 nm is still visible, which is a significant advantage for the adjustment of experimental setups.
A further result of the simulation is that for a standoff distance of 1 m a direct measurement of a 1 cm long CH4 gas column at 1651 nm is expected to be approximately more sensitive by a factor of 1000 than an indirect O2 measurement by the displacement of 1 cm background air. Therefore, for a better comparison between both methods we use 1% CH4 in N2 for direct detection.
3. Experimental Details
Gas detection by tunable diode laser spectroscopy is an established technique. We are employing the direct spectroscopy scheme. With this method, the measured absorbance spectra are fitted with calculated gas absorption lines using HITRAN line parameters. Knowing the temperature, pressure, and the absorption length, the gas concentration is obtained [
14].
For the measurements a test leak was made. This consists of a shot-blasted 100 × 100 mm2 Al-plate with a central 1 mm diameter orifice. The blasted surface ensures sufficient diffuse reflection of incident radiation. Leakage gas is ejected from the orifice at different flow rates between 1000 mL/min and 1 mL/min. A gas supply hose is connected at the back side of the plate. Flow rates and the leakage gas composition are set using a HovaCAL digital 922 SP flow controller (IAS GmbH, Oberursel, Germany).
The leak plate (
Figure 1) is mounted on a sliding stage to displace the leak position horizontally on the table. For extractive measurements, the gas is sampled by a hose with a 1 mm sampling tip mounted in a distance of 10 mm from the leak plate. The gas is pumped through a measurement cell with an optical path length of 84 cm and a volume of 175 mL. We used pump rates of a diaphragm pump between 100 mL/min and 1000 mL/min. Pressure fluctuations are minimized by an additional buffer volume between the pump and measurement cell.
For standoff measurements the laser and detector are positioned at a distance from the leak plate. The diffuse reflection of the collimated laser beam is collected by an f = 11 cm, 2” focusing lens in front of a Si-photodiode. Typically, distances of 55 cm and 52 cm of the laser with respect to the detector lens from the leak plate are used. The angle between the laser and detector beams is approximately 17°.
For static measurement, the leakage flow rates are varied in steps and the leak position is fixed at a maximum signal for extractive or standoff detection. For dynamic measurements, the leak plate is moved horizontally back and forth with a speed between 0.2 mm/s and 5 mm/s for a fixed leak flow rate, which is changed after a couple of scans.
Positive or direct detection is performed with 1% CH4 in N2. For negative or indirect detection we used 100% N2. For the CH4 measurements, a 1651 nm pig-tailed single-mode laser diode in a butterfly mount was employed (Eblana Photonics Ltd., Dublin, Ireland). For detection, an InGaAs-photodiode type G 12182-030 (Hamamatsu Photonics GmbH, Herrsching, Germany) with a 3 mm diameter was used. For the O2 measurements we used a C-mount-DFB laser diode emitting at 761 nm (nanoplus GmbH, Gerbrunn, Germany) in a custom laser housing and a quadratic 3.6 mm × 3.6 mm Si-photodiode. The lasers were driven with a standard benchtop laser current driver/temperature controller (ILX Lightwave LDC 3722, Newport Corporation, Irvine, CA, USA). Laser control, data acquisition, and evaluation were performed with a proprietary electronics board and LabVIEW (National Instruments Corporation, Austin, TX, USA).
5. Discussion
In this work, we have shown that gas leaks can be detected by the dilution of ambient O2. The fact that the leakage gas reduces the O2 concentration in the vicinity of the leak can be measured. The measurement principle is based on tunable laser spectroscopy, which was realized in an extractive and a standoff device, respectively. The method is demonstrated for N2 as the leakage gas, which is not an infrared absorber. The technique can be applied for other non-infrared absorbing gases, such as H2 or Ar, as well as for any gas, except for the ambient gas itself. Instead of O2, other infrared-absorbing background gases may be used, e.g., CO2 or H2O. However, CO2 and H2O concentrations show strong local and temporal fluctuations which have to be compensated. Consequently, an interesting application field could be an environment with a controlled atmosphere (e.g., in a greenhouse).
For static extractive detection N2 fluxes of less than 5 mL/min can be observed, corresponding to a detectable leak rate L ≥ 0.1 mbar·L/s. In consideration of a limited response speed, comparable results are obtained in a dynamical extractive detection scheme. Almost the same sensitivity level can be achieved in the case of static standoff detection from a distance of about 0.6 m. In a dynamic standoff detection scenario, only flows of 100 mL/min could be detected. The localization of the gas leak is feasible within ±5 mm. Obviously, this value depends on system parameters, such as the speed of displacement (leak), pump rate (extractive detection), or the laser spot size (standoff detection).
Comparing the direct measurements using 1% CH
4 in N
2 and the indirect measurements using dilution of the ambient 21% O
2 by N
2, the obvious result is that the sensitivity for the direct method is higher. On the one hand, the difference in the absorption line strength between CH
4 at 1651 nm (10
−21 cm
−1·mol
−1·cm
2) and O
2 at 761 nm (8 × 10
−24 bcm
−1·mol
−1·cm
2) is about two orders in magnitude [
10]. On the other hand, Si-photodiodes used for O
2 have a ten-fold higher detectivity than the InGaAs diodes needed for CH
4. This helps to reduce the effect of the large line strength difference. Our experiments indicate almost the same SNR for both methods since the influence of gas fluctuations is dominating.
For 1% CH
4 in N
2 the fluctuations of the signal with leak flux are larger than without flux (cf.
Figure 10). This effect is hardly observable for O
2 since the ambient concentration shows a higher noise level. Consequently, the detection is practically limited by the fluctuations caused by gas flow instabilities. Therefore, the estimation of leak rates L ≥ 10
−3 mbar·L/s for a 100% CH
4 standoff measurement seems to be quite optimistic. Looking at these fluctuations could be another promising method of leak detection that needs to be investigated in further experiments.
Furthermore, it is shown that the extractive method is more sensitive than the standoff one. In addition, the extractive method can be improved by optimization of the gas cell and pump rate. For O
2, a compact Herriott gas cell with an optical path length of 5 m was reported in [
17]. The sensitivity level of the above mentioned ultrasound method may be achieved by using such cell designs and leak rates <10
−2 mbar·L/s should be detectable. Even higher path lengths can be obtained by using resonant cells and corresponding detection schemes [
18,
19], which are established for high-resolution gas detection. However, for this application small changes relative to a high ambient background have to be detected. Thus, special differential cell designs or frequent fast gas exchange with ambient air as a reference gas will be required to increase the sensitivity. For the short time intervals typical for leak detection, a relative sensitivity in the O
2 concentration below 10
−4 may be detectable. This corresponds to a concentration change of 20 ppm within a 21% background concentration level.
The sensitivity of standoff techniques strongly depends on the reflection properties of the backscattering surface [
20]. A low reflectivity reduces the detected radiation intensity and the SNR. This holds for CH
4 detection at 1651 nm, as well as for O
2 detection at 761 nm. Good results are achieved with objects of high diffuse reflectivity, e.g., the reflecting plate shown in
Figure 7. The leak plate of
Figure 1a has a stronger specular reflection. However, at a scattering angle of 17° the reflectivity is similar to the value of the Thorlabs DG10-120 plate. In real applications non-cooperative specular reflectors are most difficult because they reflect in any direction. Specular reflection of common objects increases with increasing wavelength. Thus, working at 761 nm is advantageous compared to 1651 nm.
Improvement of the standoff technique might be feasible for short distances around 0.2 m to 0.3 m. Depending on the backscattering properties of leaking objects the optical beam diameter and the aperture of the receiving optics may be enlarged. Therefore, the interaction of laser radiation and the leakage gas plume relative to the total absorption path length could be increased such that minimum leak rates ≥10−2 mbar·L/s may be detectable.
In conclusion, we have shown the feasibility of gas leak detection by dilution of atmospheric O2. This indirect method has several advantages in spite of its lower sensitivity compared to direct detection of infrared absorbing gases. Since the method is independent of the leakage gas, it can be used as a universal leak sensor. For instance, a combination with another specific infrared gas detector might be possible. Compared to the established ultrasound technique, leaks can be detected which do not generate sound. Detection of visible radiation at 761 nm enables the use of fast, highly-sensitive, and inexpensive standard photodiodes. Large area detectors, special sensor geometries and arrays, are commercially available. Imaging leak detection is also feasible by the use of a laser scanning system in combination with fast data processing.
The most important application of TLS in terms of market share represents the measurement of O2. In process industries, TLS instruments from several suppliers are commercially available. As a consequence, component prices are generally lower compared to other TLS applications. In the case of O2 applications, VCSEL laser diodes can be used, which are less expensive than DFB lasers. Furthermore this laser type can be manufactured in large volumes and small packages. In this context, an integration of a laser-based O2 sensor in a mobile phone might be possible.