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Proceedings of the Combustion Institute 34 (2013) 32953301

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Electrical aspects of ame quenching

F.J. Weinberg a, D. Dunn-Rankin b,, F.B. Carleton a, S. Karnani b, C. Markides a, M. Zhai a
b a Department of Chemical Engineering, Imperial College, London SW7 2AZ, UK Department of Mechanical and Aerospace Engineering, University of California, Irvine, CA 92697, USA

Available online 23 July 2012

Abstract Carbon monoxide distributions within small laminar natural gas ames are studied by micro-probe sampling and by numerical simulation, at progressively increasing proportions of air added to a constant fuel ow. The results are compared with CO emission to the atmosphere when such ames are quenched at various heights above the burner by a variety of solid surfaces with a view to quantifying the hazard associated with, for example, domestic boilers. Numerical simulations of small ames support the experimental results. The electrical structure of quenched ames under small (<10 V/mm) electric elds is investigated, with the ultimate objective of devising a warning system signaling the onset of a quenching hazard. The variable electric eld, derived from batteries and a potential divider, is applied between the burner and a copper grid one of the quenching bodies recording current as a function of height, for both polarities. Resistance/distance is of the order 108 X/mm, depending on local temperature and composition. Because of their low mobilities, positive ions contribute only over very small distances; for longer path lengths the ame acts as a rectier. Accordingly, electron conduction is utilized to detect the proximity of a quenching surface to the ame well before any hazardous release of CO escape could arise. The contours of rst detection around the ame for a current threshold of 108 A lie substantially outside the regions in which CO is detected in quenching products for both a natural gas diusion ame and near-stoichiometric premixed ames. 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved.
Keywords: Natural gas ames; Quenching; Electrical properties; Carbon monoxide

1. Introduction The ultimate practical aim of this series of researches is to reduce the incidence of CO poisoning caused by the quenching of natural gas ames in malfunctioning burners. First, we measure CO distributions within small laminar natural gas ames using micro-probe sampling and compare the
Corresponding author.

E-mail address: ddunnran@uci.edu (D. DunnRankin).

results with predictions by numerical simulation. Next, CO ame concentrations are compared with CO emission rates to the atmosphere when such ames are quenched at various heights above the burner by a variety of solid surfaces. All the work involves progressively increasing proportions of air added to a constant fuel ow, so as to maintain a constant power input. The quenching measurements focus on compositions ranging from pure diusion ames to progressively increasing air admixtures. The reason is that such burners (e.g. boilers) are generally designed to operate under near-stoichiometric conditions and when they

1540-7489/$ - see front matter 2012 The Combustion Institute. Published by Elsevier Inc. All rights reserved. http://dx.doi.org/10.1016/j.proci.2012.07.007

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malfunction due, say, to an obstruction in the air supply, they tend to burn rich. Using variable electric elds on the order of 10 V/mm and reversible polarity, these quenching measurements are then associated with the measured current voltage characteristics. The object of applying such small voltages is to measure currents, eld intensity, and resistance distributions for positive and negative charge carriers in various quenching situations without otherwise disturbing the normal physical or electrical structure of the ames. This, nally, leads to an investigation into how the ow of charge can be employed to signal the onset of hazardous conditions, before any CO release can occur. The paper summarizes a series of hitherto unpublished (except for the preliminary study [1]) fundamental investigations, all directed towards that end. 2. Experimental All the ames were stabilized on sharp-edged 4 mm i.d., metal burners. The constant volumetric ow rate of fuel for this series of measurements was maintained at 82.75 mL/min. Composition could be varied by admixture of air with a concomitant increase in ow velocity. We have previously measured chemi-ionization and chemiluminescence in such ames [2] and found that with respect to chemi-ionization, air acts as an inert diluent to a diusion ame up to at least 75% admixture. All percentages throughout are by volume. The upper and lower limits of ammability occur, respectively, at 85% and 94.7% air addition, with premixed combustion occurring only within that range. The stoichiometric composition is about halfway in between, at 90.5% air in a mixture with natural gas. Figure 1a shows characteristic photographs of the ames we studied. This provides a height scale for the various regions of luminosity in relation to the parameters measured and their variation with air admixing. The colors are only indicative because image exposure was varied to provide a clearer view of the ame extent. CO contours in Fig. 1b, along with similar H2 measurements, were constructed from the analyses of samples extracted across axial sections by quartz microprobes; see [1] for experimental details. As a brief summary, sampling was carried out at a grid of points, along a plane perpendicular to the jet exit, by means of an approximately 0.20 mm i.d. quartz microprobe, mounted on an xyz positioner, at a suction rate of 0.039 mL/ s. Species concentrations from collected samples are then measured using an emissions console. Figure 1c shows numerically computed CO contours for both 0% and 75% admixed ames. Numerical simulations support the experimental measurements with predictions of gas-phase tem-

peratures, velocities, and neutral species concentrations. The simulations employ the cylindrical shear ow subroutine, CRESLAF, included in the CHEMKIN package [3]. Species concentrations are predicted using the GRI-Mech Version 3.0 kinetic mechanism [4]. Numerically, the burner is modeled as having a central jet with a small concentric co-ow in a 2-D axisymmetric domain. After discretizing the relevant equations, the solver, DASSL, marches axially, minimizing the residual at each height. All simulations are veried for grid-independence. For additional details regarding the simulation, see [1]. 3. Quenching Concern about CO emission initially arose from the observations of appreciable concentrations within the luminous boundaries of our ames. Figure 1b shows the loci of CO concentration (in % by volume) within ames of 0% and 75% air admixture. The results are closely paralleled by contours deduced from numerical simulation shown in Fig. 1c, which predict up to 6% CO. Although a slight spatial discrepancy exists, resulting from the lack of a heterogeneous (soot) chemistry mechanism and numerical simplications (discussed in [1]), the simulation clearly recreates the major trends of the CO prole in terms of magnitude and relative location. These results prompted the question of how much CO would escape into the atmosphere if the ame were disrupted by quenching. We studied CO release for a variety of quenching surfaces, using an exhaust system which aspirated the emerging product gasses, along with much ambient air. Multiplying the aspirated volumetric ow rate by the measured fraction of CO in the mixed gas yields the release rate of CO into the atmosphere. Once this product no longer increases with increasing aspiration rate, complete capture is conrmed. The quenching bodies: notably ame trap matrices, various metal screens held horizontally across the entire ow, and rods (simulating boiler pipes) were clamped in a vernier positioner and the height of the quenching surface above the burner was recorded for each CO measurement. The ame trap matrix consists of plane and corrugated stainless steel strips spirally wound around each other. Of the numerous results, those shown in Fig. 2 were selected to illustrate some specic aspect of quenching behavior. The matrix, which acted as a large inert metal surface, generally produced a peak at the height of the maximum ame CO concentration, implying that there it simply disrupted the ame, allowing precursor gasses to escape. This is seen in Fig. 2 along with the rather more intricate behavior of various metal grids. The grids were of approximately 55% open area, with 16 16 holes per sq. cm.

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Fig. 1. (a) Photographs of natural gas ames with no and 75% air admixture. (b) Contour lines of CO concentration (volume %) superimposed on photographs of natural gas ames with 1 mm square grid overlay. (c) CHEMKIN computed CO contour lines of methane ames. Scale units in mm.

Although the Al grid, for example, also shows a small subsidiary peak that coincides with a maximum within the ame, it is clear that, close to the burner, quenching by some metals can generate CO from the reactants in excess of the amount present in the unperturbed ame. This is not surprising since Ni and Al have been used as constituents of catalysts for the production of syngas from natural gas. It implies that the use of new alloys in boiler tubing, and also metal impurities, may need to be scrutinized from that viewpoint. We found no CO present from the products released beyond the region of luminosity see

Figs. 1a and b which extends to about 16 mm above the burner for diusion ames and some 5 mm less for near stoichiometric premixed ames. This is worth bearing in mind, since all the parameters that follow are here plotted against H, the height above the burner. The measurements imply that as much as 6% (10% at lower ow rates [1]) of the CH4 feed may be converted to CO. This is equivalent to 35 L/ min for the 30 kW recommended for a one bedroom at. During 19992004, CO poisoning caused 16,447 deaths in the United States, the principal cause being incomplete combustion in malfunctioning heaters/boilers.

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Fig. 2. Rate of CO emission to atmosphere for various quenching surfaces.

4. The electrical structure of quenched ames In order to correlate the electrical ame response with the possible release of CO during ame quenching, we applied small electric elds between the burner, as one electrode, and the copper grid, as the other. The copper gauze was chosen because its high thermal conductivity keeps it relatively cool and it proved chemically and catalytically inactive in the quenching measurements (see Fig. 2). The variable eld strengths applied were of the order of 1 V/mm, which is two orders of magnitude less than any we used previously, e.g. for saturation current measurements. Nine-volt batteries, in series of up to 10 as necessary, provided a steady potential dierence, using a potential divider and reversible polarity. The exact voltages were measured and currents, generally on the order of 107 A, were recorded using a Meterman Multimeter, as the height of the copper grid electrode above the burner was varied. The object of applying such small voltages was to measure currents, eld intensity, and resistance

distributions in various quenching situations without otherwise disturbing the normal physical or electrical structure of the ame. Theory [5] implies that, so long as the rate of charge removal by the electric eld is negligible by comparison with the equilibrium rates of ionization and recombination, the system exhibits some of the properties of an Ohmic conductor. In particular, the eld strength is simply voltage/distance, (V/x), and the number densities of positive and negative charge carriers within the plasma are equal. Their drift velocities in a eld are, of course, vastly different, and since electron mobility, K, is 23 orders of magnitude greater than that of positive ions, K+, the current is carried predominantly by electrons. The resistivity, when electrons carry all the current, can then be written as (a/js)0.5/e K, where e is the electron charge and a the recombination coecient between positive and negative charges. The saturation current density, js, has been used instead of the rate of charge generation because it is a measurable parameter. The ratio of maximum to minimum (js)0.5 measured for this range of compositions in some of our previous work [2] is indeed close to the ratio of maximum to minimum resistances per unit length, dR/ dx, listed in Fig. 4 and further discussed below. We tested for current on open circuit to assess any contributions of Langmuir probe eects. Only currents on the very limits of detection were observed, allowing any such eects to be disregarded. If we treat the inter-electrode space as being radially uniform an approximation forced upon us in any case by the grid being an iso-potential surface and by its eect on the ow pattern we can subdivide it, roughly, into four cylindrical slabs. We have: (1) the dead space in contact with the burner, (2) the reaction zone in which the charges are generated,

Fig. 3. Current as function of height of grid at two voltages and opposite polarities for natural gas ames of two compositions.

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Fig. 4. Voltage vs height such as to maintain constant current, for various compositions and both polarities. Numbers on right side of legend are dV/dx (V/mm) and dR/dx (MX/mm) for straight lines. (a) Burner negative. (b) Burner positive.

(3) the region of hot inert products, provided there is enough height, and (4) the quenching zone in contact with the grid. The maximum height of zone (3) is ultimately limited only by the grid height and by intermixing with the ambient atmosphere, the rest are xed by underlying mechanisms; zones (1) and (4) are necessarily very thin. Figure 3 shows current plotted against the height of the grid above the burner, H, for the two polarities and two compositions. The two particular voltages (chosen arbitrarily no potential divider was used) arise from four and six, nominally, 9 V batteries. In general the current increases with decreasing distance, and increasing voltage, because of the increasing eld in the ionization zone. Perhaps the most striking observation is that the system acts as a rectier as the screen electrode is lowered from above, until it encounters the reaction zone. That is, there is essentially no current detected with the burner positive until about 18 mm, which is approximately the height of the reaction zone. The resistance of the product zone when any current carried would rely on the mobility of positive ions i.e., when the burner is positive is extremely

high (the screen is too cool to emit electrons). The failure of positive ions to carry current adequately can also be seen over a much smaller distance when the burner is negative. This is responsible for the earlier decrease in current as the grid approaches the burner. Eventually, of course, quenching is complete and extinguishes the ionization source. Interestingly, the resistance calculated from these results does not tend to zero as H tends to zero. The relation of this is due to quenching and is to become the subject of further study. All the inections in the curves correlate with changes in luminosity compare Figs. 1a and 3. Despite a considerable change in overall ow rate, the curves in Fig. 3 are similar for increasing air additions and for non-ammable mixtures that burn as diusion ames. The shapes do not change much for near-stoichiometric mixtures either, but the currents approximately double. Also the height at which the blue and black curves detach from the axis decreases to about 10 mm for near-stoichiometric mixtures, coinciding with the apex of the inner cone of the premixed ame. The ux of charge is a conserved quantity. For a xed rate of ionization, current is constant as height (H) is varied. Figure 4 shows loci of con-

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stant current for various compositions and both polarities. They were obtained by incrementally increasing voltage, using the batteries in series with a potential divider, and measuring the height at which each particular chosen current magnitude was attained. This procedure ensured that along each voltageheight curve the eld strength in the reaction zone remained constant. Since compositions covered the entire range from pure fuel to near stoichiometric, rates of ionization varied widely, necessitating the use of dierent currents to be kept constant for dierent air admixtures and polarities, as listed in the legend of Fig. 4. The main interest lies in the voltage (V), electric eld and resistance (R) distributions in the hot gasses. If x is the distance coordinate along the height, H, then, dV/dx is the local eld intensity. Moreover, dividing each V prole by its (constant) current converts the prole to a measure of resistance, R, against height. The resistance gradient, dR/dx, then yields the prole of local resistance per unit height. A constant electric eld (i.e. d2V/dx2 = 0) implies a constant resistance per unit length in those regions. dR/dx, depends on the local mobility and number density of charge carriers, which in the linear regions indicates a constant product of number density and mobility. The curves of Fig. 4 indeed do tend to straight lines beyond the highly conducting reaction zones. At rst sight it may seem surprising that the burner negative and burner positive graphs are at all similar. The reason becomes clear when the extent of the height scales is compared. The rectier region due to the inadequacy of positive ions as charge carriers is absent altogether in the latter case (Fig. 4b) as the nal measurement point at which the maximum voltage is attained occurs just beyond the luminous ame tip. In both cases we are dealing with electrons passing through gasses of varying temperatures and compositions, though in opposite directions. These resistance values are consistent with conductivities measured in ames and in the hot post ame gasses [6,7]. Bearing in mind their totally dierent trajectories and tenfold ow velocity increase in going from 0% to 90% air addition, it is remarkable that the dierences are not substantially greater. The main determinant appears to be the mean gas temperature through which the electrons traverse. This is seen most clearly in the longer path trajectories in the burner negative case. As air is progressively added, the temperature passes through a minimum for mixtures short of stoichiometric [1]. This is thought to correspond to the dR/dx peak and is due to the cooling caused by additional air admixture before the stabilization of a premixed near-stoichiometric ame at the burner mouth. As the ame passes through this minimum, the knee of the curve moves from substantially above the luminous ame tip (approximately 15 mm

downstream) to close above the ame tip, approaching the behavior of the burner positive case with increased admixing. The reason why the premixed ames in Fig. 4a do not exhibit the same delayed onset of high resistivity as do the non-premixed ames probably lies in their substantially dierent ame interaction with the mesh electrode. Whereas diusion ames burn in a stagnation point ow near the mesh, which greatly increases their contact area with the electrode, the near-stoichiometric ames retain a more constant footprint and their reaction zones are more readily quenched. The burner positive case is further complicated by the cooling in the dead space in contact with the burner, as the electron trajectories converge on the narrow burner rim, well within the luminous zone of Fig. 1a. In proximity to the highly conducting reaction zones at the foot of the curves, no large potential dierences can be maintained and the gradients become very small. The idealization of radially uniform cylindrical slabs is clearly untenable where the grid electrode contacts the highly conducting inner cone of a near-stoichiometric premixed ame. The outcome of such encounters can be followed in some detail in regions below 20 V in the graphs. 5. Electrical detection of proximity of quenching surface The facility of monitoring ame solid surface interactions electrically may have a variety of applications, not necessarily linked to quenching. In the present context, however, our chief objective was its use to detect the proximity of a quenching surface to the ame, well before any hazard of CO escape could arise. All the aforegoing measurements indicate that such a warning device should be based on a negatively charged burner to utilize the farther electron penetration. Comparison of Fig. 3 with Fig. 2 already shows that as a quench detector the current with the burner negative, signals the approach to a quenching surface at a height which is more than 30 mm in excess of that at which any quenching is ever recorded. In practice, of course, quenching may occur by surfaces not directly above the ame. To explore the loci of electrical quenching detection, a rod with a rounded end was used as the positive electrode. It was clamped in the xyz positioner and manipulated to approach the ame orthogonally at locations all around the ame periphery. The contours of rst detection of a current are shown in Fig. 5 for both a pure fuel diusion ame and a near-stoichiometric premixed ame at two potentials (37 and 56 V). Interestingly, the contours are remarkably similar to each other, in spite of the

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Fig. 5. Spatial contours of initial current detection for 0% and 75% air admixture by positive probe at <108 A threshold.

circumstance that the ow rate in the latter is ten times greater. They lie massively outside the regions in which CO is seen (Fig. 1a) or detected in the products of quenching (Fig. 2). Situations may arise when such a high sensitivity is not required. In our work the threshold for current detection was 108 A and was triggered at heights approaching 60 mm, whilst no quenching was ever observed for height in excess of 15 mm. Clearly, a much lower threshold could be set should it be desirable, for example, to heat bodies by ame products in closer proximity, yet without quenching the ame. We conclude that detecting the proximity of quenching surfaces from a ame, to alert the user before any carbon monoxide is released, is feasible and requires only the use of small batteries. The detection is particularly eective in the hot post-ame region of the ow. It could readily be developed into a system which would give warning of hazardous conditions arising, say, from an unexpected elongation or change in ame shape due to, for example, an obstruction in the feed.

Acknowledgments This work is supported by NASAs ISS Research Project via agreement NNX07AB55A with Dennis Stocker as Technical Monitor.

References
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