1. Introduction
A convenient method of producing desired gaseous products and syngas in methane combustion is through partial oxidation (POx) [
1]. By isolating gaseous reactants in separate injector flow passageways, the reactants may exit, mix, react, and combust (using an external ignition source), creating a product diffusion flame [
2]. Specifically, in methane/oxygen (CH
4/O
2) POx burners, depending on the amount of fuel-to-oxidizer, or equivalence ratio (ϕ), diverse amounts of product gases may be generated. The greatest quantities of product gases from nonstoichiometric CH
4/O
2 combustion result as hydrogen (H
2), carbon monoxide (CO), water (H
2O), and carbon dioxide (CO
2). By varying reactant flow conditions, even larger amounts of H
2 may be produced and then gathered [
3]. Furthermore, if the gaseous reactants are combusted under fuel-rich, non-stoichiometric flow conditions, additional amounts of syngas may be generated in a CH
4/O
2 reaction, thereby creating gases for collection [
4]. Therefore, knowing operating regimes where highly efficient, stable CH
4/O
2 diffusion flames burn would be advantageous when producing and collecting H
2 gas.
In CH
4/O
2 fuel-rich combustion, when ϕ > 2, the primary product gases are H
2 and CO. Operating under highly fuel-rich conditions, (ϕ ~ 4) results in 60% of the combustion products being H
2. Molar fractions of products from CH
4/O
2 combustion are represented in
Figure 1, where the data presented were compiled using a chemical equilibrium analysis software, version year 1999, burning CH
4/O
2 at standard temperature and pressure (STP) conditions [
5]. Therefore, being able to burn fuel-rich CH
4/O
2 under stable flame conditions would be beneficial to H
2 collection.
During combustion, the resultant CH
4/O
2 diffusion flame may burn as a stable (anchored, torchlike profile) or unstable (detached, oscillating) flame. While work on diffusion flames has been extensive, the understanding of the exact stable flame regimes for fuel-rich CH
4/O
2 operation is not completely known. For example, in non-premixed CH
4/O
2 flow, there are numerous operating and geometric parameters that may contribute to a stable flame behavior. Some of these parameters include the reactant type, injector type, reactant initial conditions, reactant flow conditions, injector geometry, operating pressure, etc. In this research work, focus was placed on examining the effects of the injector type (single, coaxial flow), injector features (secondary annular flow impingement angle), and injector geometry (annular flow exit area), as well as their impact on the CH
4/O
2 diffusion flame behavior and flame condition with respect to the injector exit. These parameters, combined with reactant initial conditions and flow rates, will help to further progress in understanding CH
4/O
2 diffusion flame stability, not only leading to increases in H
2 collection but also advances in operation start-up and safety, burner combustion efficiency, minimization of burner downtime, and decreased soot formation [
6,
7,
8].
Studies have shown that when diffusion flames are stable and attached to the injector exit, up to 95% combustion efficiency (defined as the percentage of completely burned fuel) may be attained [
9]. When operating as a stable flame, the diffusion flame has an increased chance of anchoring itself to the injector exit. This location allows for the burning of reactants to occur directly at the injector exit plane, thereby minimizing any unburnt fuel entering the burner and escaping out the exit. Furthermore, by having an anchor point, the flame will have a decreased chance of experiencing flame blowoff conditions (i.e., flame extinction or disappearance). Hence, where and under what parameters stable diffusion flames operate is the challenge.
Reviewing previous works specifically with CH
4/O
2 diffusion flames using single coaxial injectors operating with a constant oxidizer-to-fuel mass ratio, (O/F)
mass, showed that any increase in the reactant Reynolds number (Re
D) resulted in the flame changing from an anchored flame to an unstable flame that was detached from the injector exit [
10,
11,
12,
13,
14,
15]. Outcomes from these studies were that as the reactant flow inertia rose above a critical exit velocity, the diffusion flame mixing regime required additional axial distance away from the injector exit to react and combust. Other works showed that as the gap between diffusion flame velocity and flow velocity increased, or when the diffusion flame base reached a maximum radius, the flame may result in a near-blowoff flame condition due to the imbalance of flow mixing and chemical reaction time [
11,
16,
17,
18,
19,
20,
21].
Due to the desire to achieve stable, fuel-rich burning with CH
4/O
2 for H
2 production and collection, this experimental investigation was conceived to observe the reactant flow and injector geometric parameters that influence diffusion flame stability to determine stable CH
4/O
2 diffusion flame operating regimes. The objective of this work was to establish diffusion flame stability regimes (or maps) to narrow down the influence of reactant and injector parameters that lead to stable CH
4/O
2 diffusion flames specifically from inverse shear coaxial injectors (i.e., O
2 flowed through the center, primary injector passageway and CH
4 flowed through the secondary annular flow channel). This work looked at the variation of injector flow geometry, particularly the injector secondary annular flow exit area in an atmospheric chamber environment (i.e., 1 atm) with room-temperature reactants. The secondary annular flow variation was of interest; in other studies using hydrocarbons and shear flow injectors, researchers that examined secondary flow impingement angle effects in CH
4/O
2 coaxial injectors [
1,
22] or CH
4/O
2/Ar coaxial injectors [
23] showed that injector geometry and flow velocities affect flame behavior through either additional mixing or flow breakup. These works used constant total mass flow rate and constant Re
D,O2 [
22] or constant CH
4 and Ar mass flow rates with three channel impingement angles of 45°, 60°, and 90° with respect to the injector exit [
1,
23]. The difference in this work compared to the previous literature was that a constant secondary flow impingement angle of 30° was evaluated with three different secondary annular flow exit areas in a single CH
4/O
2 inverse coaxial injector with a fixed center flow area and varying reactant mass flow rates.
Outcomes from this experimental work will provide new flame behavior results for single inverse CH4/O2 coaxial injector diffusion flames under laminar and turbulent reactant flow conditions for different secondary annular flow areas in an atmospheric pressure environment. This work contributes to the field with new diffusion flame results as a function of injector geometry and annular flow. Specific contributions from this study will be the development of flame stability region maps for CH4/O2 diffusion flames. These results may be used to identify appropriate fuel-rich burning regimes where stable, efficient flames reside. The goal of this new investigation was to aid POx burner and syngas designers in achieving stable operating flame conditions with gaseous CH4/O2 to further increase H2 production and efficient methane burning.
3. Results and Discussion
Combined, over 640 CH4/O2 experiments were conducted at the Advanced Combustion and Energetics Laboratory (ACEL) at Penn State Altoona. Diffusion flame stability regime maps were generated based upon reactant flow parameters and visual observation of the flame behavior to define the regions where each flame behavior existed for the three different injectors.
Specific flow parameters of interest for each injector examined were:
SD, for this work, was the average flame distance, which was determined from the measured distance that the base of the diffusion flame resided from the injector exit through cinematography [
36]. To capture the experimental error, the general form of uncertainty was a function of independent variables. The uncertainty error of the independent variable combined the exactness error of each instrument and measurement device, as well as the experimenter’s overall consistency, through an addition of the error, and was then used to determine the resultant (or dependent parameter) uncertainty interval using a second-power equation [
37]. In total, nine uncertainty parameters were estimated for flow diameters, temperatures, pressures, mass flow rates, and time. The resultant uncertainty interval for the flow parameters (i.e., velocity, mass flow rate, ReD, etc.) determined from this analysis was represented by the data point error bars in each of the result figures, as well as data comparison tables at a 95% level of confidence. Experimental results are provided in the subsequent sections.
3.1. Visual Diffusion Flame Observations
Throughout testing, the diffusion flame operating conditions were observed in real time using video cinematography and optical viewing windows on the experimental burner. Three clear diffusion flame conditions were seen and were identified as an anchored (stable) flame, an oscillating, detached (unstable) flame, or a near-blowoff (unstable) flame. These flame behavior classifications were also reported through visual observations using video cinematography in other diffusion flame works [
10,
11,
12,
13,
14,
23,
24,
25,
26,
27,
33,
38]. Individual time stamps during steady flow operation for each of the diffusion flame behaviors are shown in
Figure 7,
Figure 8 and
Figure 9. It should be noted that the reactant flow was from right to left in the images, and that the shadow seen near the injector exit was the camera reflection off the optical viewing windowpane.
In the flame image provided in
Figure 7, the stable, anchored diffusion flame was observed to be a blue, non-pulsing, bright diffusion flame, physically anchored to the injector exit. The flame remained attached to the injector exit during the entire portion of the experiment. The diffusion flame did not oscillate or pulse and decreased in overall length as CH
4 velocity increased until the flame was no longer anchored.
In
Figure 8, the detached diffusion flame displayed a distinct standoff distance (or liftoff height) between the flame and injector exit (seen and indicated by the portion of the image where there is no flame). During steady flow operation (i.e., reactant steady mass flow rate), the detached flame oscillated axially in the viewing plane, with the flame front occurring at numerous locations. These oscillations were either small or large axial deviations from the previous recorded frame as a function of reactant flow conditions (ϕ and secondary CH
4 annular flow velocity). The flame liftoff height was recorded and used to calculate SD (process covered in depth in the
Section 2). Overall observations indicated that as CH
4 flow velocity exceeded the local diffusion flame speed, this, in conjunction with the 30° secondary annular flow impingement angle, resulted in the diffusion flame becoming more unstable, with SD achieving greater values for greater CH
4 flows. While the three injectors evaluated in this study had different secondary annular flow exit areas, this detached flame observation with ϕ and secondary CH
4 annular flow velocity was observed in all injector cases, as well as in other single coaxial work [
10,
11,
12,
13,
14,
24]. Also, unlike the symmetric, stable, anchored flame condition seen in
Figure 7, the detached flame was asymmetric and displayed a large, blunt-shaped flame core.
In
Figure 9, a near-blowoff diffusion flame is presented. While the flame existed during the runtime, the flame itself disappeared in and out of the optical window view. This was due to the diffusion flame experiencing even greater amounts of axial fluctuations than the detached diffusion flame. The near-blowoff diffusion flame primary burning zone was housed far from the injector exit, typically in the burner exhaust duct. As seen in
Figure 9, the near-blowoff diffusion flame exhibited a yellowish/orange color, with no clear shape, indicative of less oxygen and incomplete combustion. It should be noted that despite the near-blowoff flame behavior burning downstream of the injector face, all these flame classifications were considered diffusion flames since CH
4 and O
2 were separated in the coaxial injector, reacted at a flame front [
16,
39,
40], and covered a large area over which the chemical reactions transpired [
41].
Overall, from a visual observation, anchored diffusion flames were the longest, whereas the flames became shorter when transitioning to detached and near-blowoff flames. While this work used a 30° secondary annular impingement angle, this flame length phenomenon was also seen in other studies that used no impingement angle (0°), non-premixed coflow injectors, and it may be explained by elevated (O/F)
mom, with rises in primary flow Re
D,O2 [
12,
28].
3.2. Diffusion Flame Results—Test Cases and Experimental Data Ranges
As discussed in earlier sections, three different injectors were evaluated in this study. The injectors were defined as either baseline, larger annular flow area, or smaller annular flow area. Specific geometric values are provided in subsequent sections for each injector case. As an overall evaluation and comparison, actual ranges from each test series are provided in
Table 2. It should be noted that the ranges displayed from this series of experiments listed in
Table 2 corresponded to outcomes of either anchored, detached, or near-blowoff flame conditions. Test outcomes in which no visual combustion was demonstrated (i.e., no ignition) may be outside of these reported results. In addition, a comparison table summarizing flame behavior trends across injectors is provided in
Table 3.
3.3. Diffusion Flame Results—Baseline Secondary Annular Flow Area Case
The first series of experiments examined the diffusion flame behavior using an injector designed with a secondary annular flow area of 4.79 × 10
−5 m
2. This secondary annular flow area was used as a baseline case for this investigation to provide a broad range of flow parameters and a large stability map to compare against other injectors with increasing and decreasing secondary annular flow area. In addition, this size secondary annular flow area and fixed primary flow area were used in other inverse CH
4/O
2 coaxial injector studies using the same experimental burner, but with different secondary impingement angles and flow conditions [
10]. In total, over 280 experiments were conducted with this injector.
Figure 10 represents a non-dimensional diffusion flame stability regime map, comparing reactant ϕ to Re
D,CH4. In the stability regime map, the three observed diffusion flame conditions of anchored, detached, or near-blowoff are presented. No ignition experiments are identified by blank regions of data in the flame stability regime maps.
In reviewing
Figure 10, it was observed that there were identifiable regions among the different diffusion flame classifications, with the baseline injector having a small number of experiments (<3.9%) where there was no ignition (blank regions) over the test ranges covered. The detached and near-blowoff flame types mainly resided at fuel-rich mixtures above the laminar Re
D,CH4 (>2300) condition. It was observed that for a Re
D,CH4 between 2600–4600 and ϕ > 2, the diffusion flame behavior was a combination of anchored and near-blowoff results, indicating a sensitivity to minor variances in reactant flow rates, governed by Re
D,CH4, where increases in CH
4 velocity with decreases in O
2 flow resulting in flame liftoff from the injector and a change to a near-blowoff state [
36,
42]. This overlap or scatter implies for this combination of secondary annular flow area and 30° impingement angle, the ignition of CH
4/O
2 and subsequent flame speed was able to initially anchor the flame to the retractable spark plug and then travel from the ignition location to the injector exit without being overcome by the reactant flow speed to push the flame further downstream from the ignition zone. Small deviations in either (O/F)
mass or (O/F)
mom, as shown in
Figure 10, would result in the flame igniting, but not be able to anchor to the retractable park plug and travel back to the injector exit. Any further increase in Re
D,CH4 would result in the flame being unstable. A similar trend was seen for ϕ = 1.9, where a boundary was formed between detached and near-blowoff flames, depending primarily on ϕ, not Re
D,CH4.
As CH
4 flow entered more turbulent conditions (Re
D,CH4 > 3000) and ϕ > 0.75, primarily unstable flame behaviors were observed. This led to the hypothesis that the flame velocity was not greater or equal to the CH
4 flow velocity, forcing the mixing zone (or diffusion zone of fuel and oxidizer) for the diffusion flame away from the injector exit, where flame velocity was the speed of the diffusion flame during burning and flow velocity was the velocity of the reactant at the injector exit plane. Any increase in ϕ at high Re
D,CH4 further pushed the flame downstream in the burner until the flame was a near-blowoff or eventual blowout condition. This observed flame behavior at high Re
D complements flame blowout behavior from other works [
11,
15,
19,
21].
From an injector geometry standpoint, the 30° impingement angle tended to inject the secondary annular fuel flow into the primary oxygen flow at the injector exit. This, combined with the large velocity differences under fuel-rich flow conditions, results in the shear mixing at the injector exit being disturbed, which is a different outcome from 0° shear coaxial injectors, where velocity variances enhanced reactant mixing by introducing fresh reactants at the injector exit [
2,
32]. In the lower regions of the diffusion flame stability regime map, when the flow conditions were fuel-lean (ϕ < 0.5), it was observed that the diffusion flame was an anchored flame. The combination of a lower secondary annular flow velocity and 30° impingement angle for ϕ < 0.5 flows was able to maintain a sufficient reactant mixing zone for combustion at the injector exit.
Figure 11 shows the X
STO with values ranging from 1.62 to 19.81. The maximum X
STO value occurred at a Re
D,CH4 of 7358 for ϕ = 1.86 for the baseline secondary flow area 30° impingement angle injector experiments.
In
Figure 11, ϕ data were presented in ranges to accommodate not only uncertainty error but also allow for increased data points where individual ϕ may have had just one data point at the exact ϕ value. From
Figure 11, it was observed that the baseline injector detached flame regime covered a wide range of ϕ and Re
D,CH4. The more fuel-rich the flame, the farther away from the injector exit the diffusion flame operated. This was due to the breakup of the reactant streams, forcing the mixing of the reactants and combustion zone further away from the injector exit. This disturbance of the reactant streams was due to the increase in the amount of high-speed turbulent fuel flow in the annular stream penetrating the primary oxygen flow. X
STO increased with Re
D,CH4, with the greatest X
STO occurring for the largest recorded ϕ value. For the particular Re
D,CH4 tested range, any increase in ϕ beyond 1.86 or X
STO beyond 19.81 resulted in a near-blowoff flame due to the diffusion flame becoming more unstable from the increase in CH
4 velocity, a phenomenon also witnessed in 0° coflow work [
23].
3.4. Diffusion Flame Results—Larger Secondary Annular Flow Area Case
The next series of experiments examined the diffusion flame behavior using an injector designed with a larger secondary flow area of 8.09 × 10−5 m2. This specific secondary flow area size represented an increase in the secondary flow area of 68.8% compared to the baseline case while maintaining a 30° impingement angle and the same constant primary flow area.
The three flame cases for the 210 experiments conducted are presented in a non-dimensional flame stability remine map comparing ϕ to Re
D,CH4, as shown in
Figure 12.
Based upon
Figure 12, compared to the baseline injector, the 68.8% increase in secondary annular flow area resulted in a decrease in the number of no-ignition tests (<2.3%) and a larger percentage of observed cases of stable, anchored flames. Unlike the baseline case, anchored flames were observed in the region of Re
D,CH4 < 4000 for high fuel-rich combustion (ϕ > 2), as well as all tested laminar flow (Re
D,CH4 < 2300) for any ϕ value. The combination of the 30° impingement angle and decreased CH
4 exit velocities from the increased secondary annular flow area further promoted mixing near the injector exit compared to the baseline case. It is hypothesized that this combination allowed mixing to occur closer to the injector exit plane in addition to providing a greater annular column of CH
4 to react with the same O
2 jet amount.
Like the baseline injector, the detached and near-blowoff flame conditions seen in
Figure 12 tended to gather and burn at higher ϕ and Re
D,CH4. A distinct boundary was observed between a detached and near-blowoff flame at ϕ = 1.93; dependent on ϕ, but independent of Re
D,CH4, even as Re
D,CH4 increased from 4200.
It was observed that at a ϕ > 1.94 and Re
D,CH4 of 4200, a region of mixed anchored and near-blowoff flame behaviors existed. Any minute changes to Re
D,CH4 resulted in a transition from one flame behavior to another, skipping over a detached flame case. This implied a sensitive boundary for this injector, with any increase in fuel velocity resulting in large SD oscillations and a quick transition to a near-blowoff condition [
32,
36]. Like the baseline injector, all three flame types were observed at Re
D,CH4 between 4000 and 4400, with near-blowoff flames appearing in the majority at ϕ > 2. Compared to
Figure 10 for the baseline injector, clear flame regimes were once again identified between each flame type.
Figure 13 shows X
STO for the larger secondary annular flow injector case ranging from 3.01 to 19.47, with the maximum X
STO occurring at a Re
D,CH4 of 6859 for ϕ = 1.88. Comparing
Figure 11 and
Figure 13, detached flames from the larger secondary annular area injector initially resided farther away from the injector, with the closest being an X
STO of 3.01 (compared to 1.62 of baseline data). Any ϕ beyond 1.88 in this range of Re
D,CH4 resulted in a near-blowoff flame. Among the ϕ ranges, X
STO increased slightly with Re
D,CH4, with the greatest X
STO also occurring for the detached diffusion flame with the largest recorded ϕ value. Compared to the baseline injector design, the larger secondary annular flow area injector experienced the lowest X
STO maximum value, as well as having fewer detached flames below Re
D,CH4 < 4000.
3.5. Diffusion Flame Results—Smaller Secondary Annular Flow Area Case
The last series of experiments examined the diffusion flame conditions for an injector designed with a smaller secondary annular flow area of 2.75 × 10−5 m2. This specific secondary flow annular area size represented a decrease in the secondary flow area of 42.5% compared to the baseline case while maintaining a 30° impingement angle and the same fixed primary flow area.
The three flame cases for the 150 experiments conducted are presented in a non-dimensional flame stability map comparing ϕ to Re
D,CH4 shown in
Figure 14.
Based upon
Figure 14, it was observed that there was a large portion of the flame stability regime map that had blank space or no reported combustion data (2500 < Re
D,CH4 < 6400 and ϕ > 2.6). This space represented fuel-rich operating conditions where there was no discernible flame or any ignition after the spark igniter was initiated. With a smaller secondary annular flow area, CH
4 velocity was considerably faster compared to the other injector cases studied, which may explain not only why the flame did not ignite in the indicated region, but also the earlier transition (when ϕ > 1.8) to a near-blowoff flame as the reactant mixture became more fuel-rich at Re
D,CH4 above 4400. Overall, there were 16 experiments in this region that exhibited no ignition conditions. Like the other injector cases, the detached and near-blowoff flame conditions tended to occur at higher ϕ and Re
D,CH4, with the smaller secondary annular flow area injector having the fewest stable, anchored flame cases for highly fuel-rich operating conditions (ϕ > 2). Also, when compared against the other injector cases for Re
D,CH4 < 4000, there were significantly fewer stable flames and more no-ignition outcomes for the smaller secondary annular flow area injector, signifying that insufficient mixing between CH
4 and O
2 at the same O
2 jet amount occurred.
Although the 30° impingement angle tended to drive the secondary CH
4 annular flow into the primary O
2 flow compared to a shallower angle or 0° angle, the increased CH
4 exit velocity from a smaller D
H at the same CH
4 mass flow rates and ϕ as the larger D
H injectors led to breaking up the primary O
2 core. This flow disturbance at the injector exit led to the reactants meeting further downstream, or even not at all. As seen in
Figure 14, the unstable diffusion flame regions dominated operations above stoichiometric conditions, where increased amounts of CH
4 flow resided. As ϕ and Re
D,CH4 increased, the diffusion flame became even more unstable, leading to a near-blowoff state or no ignition.
When comparing the stability maps among the three different injectors, it was observed that as the reactant mixture became more fuel-rich (ϕ > 1), the greater the secondary annular flow area, the greater the chance for an anchored, stable flame. Overall, among the three different injector secondary annular flow areas, it was observed that an increase in secondary CH
4 annular flow velocity resulted in a decrease in stable, anchored diffusion flames due to the mixing and reaction zone being disrupted at the injector face and reactant flow velocities being greater than the flame velocity. This annular flow velocity trend was also observed in CH
4/O
2 studies with straight (0° impingement angle) coaxial injector flow, further emphasizing that the diffusion flame is influenced by high-speed annular fuel flow, leading to unstable flame conditions [
29]. For a larger secondary annular flow area, the CH
4 velocities were smaller at the same ϕ compared to the other injector cases studied, thereby allowing the flame speed to keep up with the reactant flow velocities and stay attached to the injector face. This trend was also observed in a diffusion flame stability study with a larger secondary annular flow impingement angle [
10]. For POx reactors, when looking to produce substantial amounts of H
2 in a shorter amount of time, the larger secondary annular flow area with a 30° impingement angle coaxial injector would, therefore, be best at higher flow rates. Compared to coaxial injectors that used greater secondary flow impingement angles [
1,
23,
24], the 30° secondary annular impingement angle showed agreement in that the larger the annular exit area and the lower the flow velocities, the less chance of flow breaking up and the more stable the diffusion flame. In addition, it was observed that the location of the flame core for this work also increased with the increase of O
2 flow rate, as seen in 45◦ [
1] and 60◦ impingement angle cases, albeit surrounded by an Ar sheet [
23]. However, the sharper the secondary flow impingement angle with the primary flow [i.e., 45°] for the same injector geometry, the greater the chance for a stable operating flame under the same initial flow conditions [
24].
Figure 15 shows X
STO for the smaller secondary annular flow injector case, ranging from 1.95 to 24.21, with the maximum X
STO occurring at a Re
D,CH4 of 7795 for ϕ = 1.73. Any ϕ beyond 1.73 in this range of Re
D,CH4 was not a detached flame. It should be noted that for the smaller secondary annular flow area injector, there were no observed detached flames operating for ϕ beyond 1.73, whereas the baseline injector and larger secondary annular flow injector experienced detached flames for this operating condition.
As can be seen from
Figure 11,
Figure 13, and
Figure 15, the smaller secondary annular flow injector case experienced the largest maximum X
STO. In addition, this was accomplished with the lowest ϕ among the three injector cases. Comparing average X
STO values at a set Re
D,CH4 and range of ϕ, the smaller secondary annular flow area injector had higher X
STO magnitudes than the other injector cases. This result may be from the combination of the 30° impingement angle and the greater CH
4 exit velocity mixing with the primary flow further downstream from the injector face. Also, as seen in
Figure 14, there were no detached diffusion flames for this injector case at ϕ > 1.8; the impingement angle and CH
4 velocity were too great and resulted in a near-blowoff or no ignition flame.