Аннотация (русский):
The main objective of this book is to acquaint the reader with the main modern problems of the multisensor data analysis and opportunities of the hyperspectral shooting being carried out in the wide range of wavelengths from ultraviolet to the infrared range, visualization of the fast combustion processes of flame propagation and flame acceleration, the limit phenomena at flame ignition and propagation. The book can be useful to students of the high courses and scientists dealing with problems of optical spectroscopy, vizualisation, digital recognizing images and gaseous combustion. The main goal of this book is to bring to the attention of the reader the main modern problems of multisensory data analysis and the possibilities of hyperspectral imaging, carried out in a broad wave-length range from ultraviolet to infrared by methods of visualizing fast combustion processes, propagation and flames acceleration, and limiting phenomena during ignition and flame propagation. The book can be useful for students of higher courses and experimental scientists dealing with problems of optical spectroscopy, visualization, pattern recognition and gas combustion.

Ключевые слова:
Remote measurements, optoelectronic methods, multisensor data analysis, hyper spectral shooting, ramjet engine, Catalytic Stabilization

A cellular mode of combustion of a 40% mixture of hydrogen with air in the presence of platinum wire and foil in the range of 270-350 0C at atmospheric pressure was found. Time and coordinate, and color high-speed filming, combustion cells caused by catalytic instability have been experimentally detected for the first time by using the methods of routine and 4D optical spectroscopy, which allows registering the intensity of the optical spectrum simultaneously depending on the wavelength. It was found that the cellular mode is determined by the catalytic combustion of hydrogen on Pt containing particles formed during the decomposition of unstable platinum oxide in the gas phase. It is shown that the temperature dependence of the delays of hydrogen ignition on a platinum wire and foil in both stationary and rotating gases corresponds to an activation energy of 19 ± 3 kcal/mol, which is close to the activation energy of branching of the reaction chains of hydrogen oxidation. Key words: hydrogen oxidation, platinum wire, foil, ignition delay, catalytic instability, platinum oxide The development of the technology of catalytically stabilized CS combustion requires the development of catalysts with increased activity (the temperature of reaching 50% conversion should be less than 450 0C) and thermal stability. This requires an understanding of the nature of catalytic surface processes, knowledge of the detailed low-temperature homogeneous kinetic mechanism and its relationship with the mechanism of heterogeneous chemical transformations. The homogeneous ignition in a catalytic reactor threatens the integrity of the catalyst and the reactor (and can cause their destruction), therefore the possibility of preventing such an event is of primary interest for the design of the CS reactor. Ignition in the gas phase is determined by the interrelation of heterogeneous and homogeneous factors (catalytic fuel consumption, adsorption / desorption reactions involving radicals). Therefore, reliable control of homogeneous ignition requires knowledge of the combustion mechanism in the presence of a catalyst. Turbines in which natural gas is the main fuel, but natural gas combustion is stimulated by hydrogen in the presence of a CS catalyst are of particular interest [1]. The addition of small amounts of H2 to natural gas increases the efficiency of the catalyst, stabilizes combustion and prevents flame pulsation. Therefore, knowledge of the features of catalytic combustion of hydrogen is an important step for understanding the stimulating effect of hydrogen in the combustion of hydrocarbon fuels [1-6]. In [3], relatively long ignition delays were found in a 40% H2 - air mixture over a Pt foil at a total pressure of 1 atm. It was found that the ignition of H2-air mixtures at atmospheric pressure begins with the appearance of a primary combustion center at the most chemically active surface area, which initiates the propagation of the flame in the reactor. In addition, as shown in [7], the introduction of a platinum wire into the reactor eliminates the phenomenon of a negative temperature coefficient (the nature of which is still unclear) during combustion of a stoichiometric mixture of n-pentane. Air, while platinum wire has no effect on the delay time of the thermal ignition of the mixture at lower temperatures. It follows from the above that in the understanding of combustion processes over catalytic surfaces at the present time there are quite a lot of “white spots”. This Chapter is devoted to the detection and determining of the reasons for the instability of the spatial propagation of a mixture of 40% H2 - air in the presence of platinum foil or wire using high-speed color photography, routine optical and 4D spectroscopy. It discusses also the establishment of the temperature dependence of the ignition delay times of this mixture in a heated reactor at 1 atm. in a static rapid bypass plant. Experimental part Two installations were used for the experiments. In the first setup (setup 1), hyperspectrometers and a high-speed color camera were used to register the radiation. The presence of a hyperspectrometer made it possible to carry out 4D measurements (recall that 1-time, 2-wavelength, 3-spectrum intensity at a given wavelength, 4-coordinate of the emitting fragment of the light source are recorded). This setup was used to carry out experiments to analyze the optical spectra of cellular combustion of hydrogen over a platinum surface. An STE-1 spectrometer with crossed dispersion was used on the second setup (setup 2) for the traditional registration of radiation, followed by recording the spectrum with a SONY DCR-SR200E video camera, sensitive in the wavelength range of 420–900 nm. It was processed then using the Hesperus 3.0 program. This setup was used to carry out experiments to find out the nature of the 552 nm emission band, which is often recorded in combustion processes. Installation 1 (Fig. 1, 2) [8-11] consisted of a heating reactor 1, an electromagnetic valve 2, a buffer storage capacity 3, a cylinder with a gas mixture 4, a hyperspectrometer 5, a digital video camera 6, a rotating mirror 7, internal asbestos insulation 8, heater 9, external asbestos insulation 10, optical window 11, pressure sensor 12, ADC converter and computer for receiving and accumulating data 13, millivoltmeter for taking readings of thermocouple 14, aluminum ring to prevent gas circulation 15, spark ignition circuit 16, LED 17. The line in red along which the 4D spectral survey was carried out in fig. 2b. The width of this line is about 1 mm. The blue circle marks the node for tangential gas injection into the reactor. The heating reactor 25 cm long and 12 cm in diameter was made of stainless steel and equipped with a tangential gas inlet (marked with a blue circle in Fig. 2 a, b), collapsible covers, and an optical quartz window. An aluminum ring with an outer diameter of 11.2 cm and an inner diameter of 11 cm was introduced into the reactor perpendicular to the gas flow in experiments where it was required to avoid gas circulation due to the presence of a tangential inlet (Fig. 2). The temperature measurement accuracy was 0.3 K. An electromagnetic valve was used to open and close the gas pipelines. The reactor evacuated and heated to the required temperature was filled through the valve with a gas mixture from the high-pressure buffer storage capacity to the required pressure. Due to the sharp pressure drop in the buffer storage capacity and the reactor, a gas eddy arises after the solenoid valve is triggered in the reactor, leading to a reduction in the time required to establish a uniform temperature distribution [8]. As already mentioned, to prevent gas circulation, an aluminum ring was introduced into the reactor perpendicular to the gas flow. Fig. 1. Installation 1, photograph of the experimental installation It should be noted that direct measurements of the dynamics of temperature changes in the center of the reactor using thin thermocouples were performed under similar conditions in [8]. In this work, it was experimentally shown that the heating time of the gas mixture did not exceed 0.3 s. The formula, which takes into account only the convective heating of the gas mixture, gives a heating time of the order of several tens of seconds [9]. Fig. 2. Installation 1, a) - diagram of the experimental installation; b) - diagram of the reactor. In the present work, the pressure during admission and combustion was recorded using a "Karat-DI" tensoresistive sensor, the signal from which was fed through an ADC to a computer. At the moment of opening the solenoid valve, a light-emitting diode was switched on. Its radiation was recorded by a movie camera. This moment was taken as the origin of the ignition delay period, which made it possible, independently of pressure measurements, to determine its duration from a sequence of frames for each individual ignition. The flame velocities were determined from the change in the visible radius of the spherical flame, from which the apparent speed was calculated. The magnitude of the degree of expansion of the combustion products was determined, as in § 1 of Chapter 3, by the value of the maximum pressure developed during the combustion of the mixture [6]: The magnitude of the normal propagation velocity was determined from the relation [6]. A Pt foil 12 × 6 cm2 in size, with thickness 0.3 cm or a Pt wire 15 cm long, and 0.3 cm thick was placed in the reactor of setup 1. Before each experiment, the reactor was evacuated to 10-1 mm Hg. The pressure in the reactor was recorded with an exemplary vacuum gauge, and in the buffer storage capacity with an exemplary pressure gauge. Gases (hydrogen, oxygen, methane) were reagent grade Pt purity was 99.99%. The combustion process was recorded with an STE-1 spectrometer equipped with a SONY DCR_SR200E color video camera, or with a 4D spectrometer (hyperspectrometer) through an optical window in one of the removable covers (Fig. 1). Experiments on high-speed filming were carried out with gas mixtures of 40% H2 + 60% air in the range 270 - 350 0C without gas circulation. In this work, both video recording of combustion was carried out with a color high-speed film camera Casio Exilim F1 Pro (frame rate - 300 - 1200 s-1) through an optical quartz window (the resulting video file was recorded in the computer memory and then processed frame-by-frame) and registration with a hyperspectrometer combustion process (Fig. 2a). Then the obtained data were compared. The measurements were performed using VID-IK3 hyperspectrometers [14, 15] and its modified version (the photodetector array was rotated in it, and due to this, it became possible to programmatically control the angle of view and, accordingly, the frame rate). The appearance of both devices mounted on a rotary device is shown in Fig. 3, and the construction (the same for both devices) is presented in Chapter 2. The optical layout of the hyperspectrometer and the results obtained are discussed in Chapter 2. The VID-IK3 hyperspectrometer has a better spectral resolution, and the modified VID-IK3 hyperspectrometer has a better spatial and temporal resolution. The use of two devices at once made it possible to reveal new features of the hydrogen combustion process over the platinum surface. Fig. 3. Location of hyperspectrometers for studying flames: a) - VID-IK3 hyperspectrometer, 2 - VID-IK3 hyperspectrometer (modified), 3 - rotary device, 4 - Casio Exilim F1 Pro video camera on a tripod, 5 - rotary mirror with an image of the optical window of the reactor , 6 - bypass volume; b) - a block of hyperspectrometers on a rotating device. For comparison of hyperspectrometers, we present RGB hyperspectral images recorded by these devices during the combustion of a mixture of 40% H2 - air (T0 = 320 °C, P0 = 1 atm, initiated by a Pt wire (Fig. 4). Fig. 4. Comparison of RGB hyperspectral images obtained by different hyperspectrometers: a - modified VID-IK3; b - VID-IK3 hyperspectrometer. To demonstrate the capabilities of the VID-IK3 hyperspectrometer, we present the dependences of the intensity of the combustion spectra of a 40% H2 - air mixture initiated by a Pt wire on the wavelength for different points (Fig. 5) on the position on the registration line (red line in Fig. 2a) and on time (Fig. 6). Fig. 5. Dependence of the emission spectra of combustion of a 40% H2 - air mixture, initiated by a Pt wire, on the position on the red line. The initial temperature is T0 = 320 °C, P0 = 1 atm. As indicated above, since the time dependence for the combustion processes under study is quite smooth, and the spectral resolution of the VID-IK3 hyperspectrometer is two times better than that of the modified VID-IK3 hyperspectrometer. Then experiments on the study of the combustion Fig. 6. Time dependence of the combustion spectra of a 40% H2 - air mixture initiated by a Pt wire. T0 = 320 0C, P0 = 1 atm of a mixture of 40% H2 - air, 320 °C, 1 atm initiated by Pt was measured with a VID-IK3 hyperspectrometer. To establish some spatial features on the hypercube, a modified VID-IK3 hyperspectrometer was used. To diagnose dusty structures, particles emitted by a platinum wire when it was heated in atmospheric air were illuminated with a flat laser beam (“laser knife”), the shifting of which was no more than 200 μm. For visualization of solid particles, a semiconductor laser = 532 nm was used. The diagram and photographs of setup 2 are shown in Fig. 7. Here: 1 - stainless steel reactor 15 cm long and 13 cm in diameter, equipped with an optical window 8, 2 - rotary mirror, 3 - collimator with holder, 4 - spectrometer STE-1 with crossed dispersion, 5 - spectrometer entrance slit, 6 - SONY DCR_SR200E video camera, 7 - spectrometer output window. Fig. 7. Installation for registration of radiation spectra by optical spectroscopy. a) - block diagram of the installation; b-d) - photographs of the installation units.  Results and discussion of experiments Installation 1 was used to study the spatial development of ignition of mixtures of 40% H2 - air at a pressure of 1 atm. It should be noted that the ignition temperature of H2-air mixtures at 1 atm in a reactor containing Pt foil [3] is ~ 1700 lower than in a stainless steel reactor. It should be noted that the transition through the critical ignition condition is accompanied by a significant increase in the ignition delay period  only over the catalytic Pt surface. When ignited over stainless steel,  does not exceed 0.5 s and changes abruptly in a very narrow temperature range of ~ 1 degree. The retention periods in a 40% hydrogen-air mixture can reach tens of seconds both at temperatures less than 260 °C and above the “fresh” surface of the platinum foil. It is believed that the state of the “fresh” surface is realized in each initial (first) experiment, in which Pt is not pretreated with active centers of ignition. A sequence of video images of the development of ignition of a mixture of 40% hydrogen with air for various initiation conditions is shown in fig. 8. As seen from Fig. 8a, a smooth homogeneous flame is observed during ignition initiated by a spark discharge at room temperature of the walls of the reactor, in the case of a stainless steel surface. As shown in fig. 8b, if the Pt foil is placed in a stainless steel reactor, the flame front is also almost uniform. However, in the presence of a Pt wire (Fig. 8c), a cellular flame structure is observed. Before and after ignition, the Pt wire is heated due to catalytic reactions on the Pt surface. The addition of 15% CO2 to the combustible mixture ensures complete suppression of the cellular combustion mode (Fig. 8d), while the 15% addition of helium practically does not affect the cellular combustion mode (Fig. 8e). The results of a qualitative assessment of the flame velocities from the change in the visible radius of a spherical flame according to the equation given in the Experimental part is shown in fig. 9. It can be seen from fig. 9 that with spark initiation in a mixture diluted with carbon dioxide, a constant flame velocity is achieved after a certain time interval corresponding to the formation time of a stable flame front (FF) [16, 17]. However, in the presence of a platinum catalyst, as can be seen from Fig. 9, a constant flame speed (within the experimental error) is achieved almost immediately. In other words, the catalytic action of platinum leads to a sharp reduction in the time of formation of a stable FF. In addition, it can be seen from this figure that the normal flame velocity in the presence of a catalytic surface is noticeably higher (≈ 2.6 m/s) than under conditions excluding the action of the catalyst (upon initiation by a spark discharge, ≈ 1.9 m/s, in the presence of 15% CO2, ≈ 1.8 m/s). The obtained values of normal velocities (without catalyst) agree within the error with the literature data [17]. On the other hand, it is known that the speed of a laminar flame does not depend on the energy of the initiation source if the initiation energy is low (the so-called weak initiation [6]). Thus, the obtained experimental result requires an explanation. Let us turn to the facts known from the publication. In [2] some experimental facts related to the reaction between platinum (the most effective catalyst for the combustion of hydrogen and hydrocarbons) and oxygen at temperatures up to the melting point of platinum are considered. In [2] it was found that a thin film of thermally unstable solid platinum oxide (more likely, platinum dioxide PtO2, or PtO [3]) is formed in air or oxygen at room temperature [4] on the surfaces of a Pt wire or thin foil and. It thickens with an increase in temperature to about 500 0C. However, when this temperature is exceeded, it disproportionates with the formation of a metal [5]. Therefore, the weight loss of platinum in an oxic environment at elevated temperatures (470-540 °C) is explained by the formation of volatile platinum oxides, followed by the deposition of platinum on colder surfaces as a result of the decomposition of oxides. This is shown in the illustration (Fig.1) given in [2]. It shows a platinum-containing layer on a lining brick of a CS reactor, recovered after long-term operation. It can be seen from the illustration that a black oxide film is deposited at cooler edges, and crystalline platinum is deposited at a hotter surface. This means that molecules or clusters of both platinum oxides and platinum metal exist in the gas phase at temperatures above 500 °C. Therefore, Pt-containing particles diffusing into a content containing a combustible gas (for example, into a hydrogen-air mixture), for example, during the heating of a Pt wire, are catalytic centers on which hydrogen can be ignited directly during the propagation of the flame front. Fig. 8. Sequences of video images of the spatial development of the combustion process. The numbers on the frame correspond to the sequential number of the video image: (a) ignition of a mixture of 40% H2 + 60% air at a reactor wall temperature of 200 °C, initiated by a spark; 600 frames/s; P = 1 atm; there is no platinum in the reactor; (b) ignition of a mixture of 40% H2 + 60% air at a reactor wall temperature of 247 0C; Pt foil is placed in a reactor. (c) ignition of a mixture of 40% H2 + 60% air at a reactor wall temperature of 316 0C; The Pt wire is placed in a reactor. It can be clearly seen in frames 1, 61. It is also seen from these frames that the Pt wire is heated before and after the explosion due to catalytic reactions on the Pt surface; (d) ignition of a mixture of 85% (40% H2 + 60% air) + 15% CO2 at a reactor wall temperature of 320 0C in the presence of a Pt wire; (e) ignition of a mixture of 85% (40% H2 + 60% air) + 15% He at a reactor wall temperature of 309 0C in the presence of a Pt wire. Fig. 9. The dynamics of the increase in the radius R of the front of the laminar flame, calculated from the increase in the visible radius of the flame front from the data in Fig. 8: experiments a; b; c; P0 = 1 atm, 600 frames/s. Consequently, one can expect the appearance of an unstable FF caused by catalytic centers distributed in the gas phase while the combustion of hydrogen initiated by a Pt wire. This instability should be observed under those conditions in which there is no thermal diffusion instability (the composition of the combustible mixture is close to stoichiometric [6]). Let us recall that thermal diffusion instability is observed in flames in which the rates of heat transfer and diffusion are different, i.e. Le ≠ 1 (Lewis number Le = D/, where D is the diffusion coefficient of the component that determines the combustion process,  is the thermal diffusivity). Such instability leads, for example, to the cellular nature of the propagation of flames in poor hydrogen-air and hydrogen-oxygen mixtures. In this work, a cellular regime is discovered and investigated, which is not associated with thermal diffusion instability. The experimental data presented are in agreement with the experimental fact [2,4,5], indicating that the oxide layer on a bulk Pt sample with a lower surface-to-volume ratio is thinner than on a Pt wire, for which the surface-to-volume ratio is , obviously, is larger. Therefore, the number of Pt particles in the volume during heating of a massive sample is not high enough to affect the structure of the flame front. We investigated the behavior of a heated platinum wire in an oxidizing atmosphere (air) under various conditions (Fig. 10) for a clearer illustration of the above in the next series of experiments. The results of visualizing the process of heating a Pt wire with a current of 2A is demonstrated in fig. 10a. For this purpose, the wire was illuminated with a vertical flat “laser knife” (see Experimental part). It can be seen from fig. 10a that ultradispersed particles evaporate from a platinum wire when heated, which are platinum oxide, according to the literature data [2-5]. Fig. 10. Behavior of heated platinum wire under various conditions: a) heating the Pt wire (current 2A). The wire is illuminated with a vertical flat “laser knife”. 60 frames/s; b) ignition of a mixture of 40% H2 + 60% air initiated by a heated Pt wire at a reactor wall temperature of 200 °C; c) ignition of a mixture of 40% H2 + 60% air at a reactor wall temperature of 316 0C in the presence of a Pt wire. It is obvious that in the experiment on the initiation of the ignition of hydrogen by Pt with a wire in a heated reactor during a delay period of 3 ÷ 70 s under our conditions, ultradispersed platinum oxide can propagate up to ignition throughout the entire volume of the reactor. The registration of the evaporation of platinum oxide from the wire is carried out at a rate of 60 frames per second is its reason. In a “cold” reactor (Fig. 10b), i.e. when the ignition of a 40% H2 + 60% air mixture is initiated by heating a Pt wire at a reactor wall temperature of 200 °C, platinum oxide does not have time to distribute evenly throughout the reactor before ignition, since the delay time of thermal ignition is already hundredths of a second. In this regard, under these conditions, the cellular combustion mode is practically not manifested, to the same extent as in a heated reactor (compare Fig.10b and Fig.10c). Fig. 11. RGB hyperspectral images: a) combustion of 40% hydrogen in air, initiated by a platinum wire, b) combustion of 40% hydrogen in air, initiated by a spark discharge. The question of the mechanism of the participation of ultradispersed Pt particles in combustion, as well as the determination of the features of hydrogen combustion in the presence of platinum, was solved experimentally using 4D spectroscopy. Thanks to this method, it is possible to record optical spectra of radiation from a given point in space at facility 1, as well as routine optical spectroscopy at facility 2. RGB of hyperspectral images of the investigated combustible mixtures: 40% hydrogen + air upon initiation by a spark discharge [15], 40% hydrogen + air upon initiation with a platinum wire are shown in Fig. 11 a, b. In fig. 11 a, b, the window axis (x-axis) corresponds to the red line in Fig. 2a, and the y-axis corresponds to the dependence of the combustion process on time. Each line along the y-axis in Fig. 11 corresponds to one frame of information accumulation on the photodetector matrix of the hyperspectrometer (300 frames/s). A comparison of the optical emission spectra of a hydrogen flame initiated by a platinum wire and recorded along a vertical line along the diameter of the optical window (red line, Fig.2a), and a spark discharge is demonstrated in fig. 12a. Let us preliminarily point out that the hydrogen flame at low pressures is practically invisible. The reason to this is that its radiation is mainly due to the radiation of hydroxyl radicals ОН А2–X2in the ultraviolet region at 306 nm [18]. Attention is drawn to the features of the flame spectrum (Fig. 12 a, b) in the visible region, namely the system of emission bands in the range of 570 - 650 nm, which makes the hydrogen flame visible at elevated pressures, along with the lines of sodium atoms (581 nm) and potassium (755 nm), inherent in all hot flames [18] and in this case emitted from the region filled with combustion products. In [15], we showed that the bands in the region of 600 nm in a hydrogen flame, according to the data of [19], relate to the radiation of water vapor. In Table 4 from [19], cited in [15], the assignment of the bands in Fig. 12a (black curve, see also Fig. 4d) to water vapor, which is a product of the hydrogen oxidation reaction. Thus, the observed spectral lines belong only to the reaction products. It can be seen from fig. 12b and 12c, which show the combustion spectra of a mixture of 40% H2 - air, (T0 = 320 0C, P0 = 1 atm) in the range 550 - 650 nm, recorded after initiation with a platinum wire, deployed along the vertical x axis of the reactor, and the dependence of the maximum values of the spectrum intensity for a wavelength of 622 nm from the x coordinate along the vertical axis of the reactor, that at the selected time instant two maxima are recorded at x = 488 and x = 503 along the x axis, located between the spatial coordinates with relative values of 485 and 510. This means that combustion in space is inhomogeneous, otherwise the intensities of the spectral lines would change smoothly in the direction of decreasing or increasing coordinates. In other words, 4D spectroscopy makes it possible to register combustion cells, as was done above by high-speed filming (Fig. 8c, f; Fig. 10c). The experimenter may questioned whether the observed maxima in Fig. 12c with various noises, namely read noise, dark noise, quantization error or shot effect. Fig. 12. a) - comparison of the spectra of hydrogen combustion initiated by a spark discharge. 40% H2 - air, 20 °C, 1 atm (black curve) and initiated by a platinum wire. 40% H2 - air, 320 °C, 1 atm) (red curve). b) - combustion spectra of a mixture of 40% H2 - air, 320 °C, 1 atm in the range 550 - 650 nm, recorded after initiation with a platinum wire, deployed at the moment corresponding to frame 2 in Fig. 5c, along the vertical x-axis of the reactor (red line in Fig. 2a). c) - dependence of the maximum value of the spectrum intensity for a wavelength of 622 nm on the x coordinate along the vertical axis of the reactor. Fig. 13. Dependences of the glow intensity of the combustion of a mixture of 40% H2 - 60% air in the range 550 - 650 nm, recorded after initiation with a platinum wire, T0 = 320 °C, P0 = 1 atm. Among these problems, the most important is the shot effect, since in our case it exceeds the other noises in intensity by orders of magnitude. However, special experiments have shown that the shot effect does not significantly affect the features of the behavior of the spectra shown in Fig. 12c. Primary data are shown in Fig. 13. The foregoing is confirmed by the fact that the luminescence inhomogeneities caused by the catalytic instability of the phase transition are recorded not only by the high-speed filming method (Fig.8c), but also by a hyperspectrometer (the same experiment, Fig. 14) directly on the hypercube. Indeed, it can be seen from Fig. 14 that when measured with a modified VID-IK3 hyperspectrometer on a combustion hypercube of a 40% H2 - air mixture (T0 = 320 °C, P0 = 1 atm), bright spots (hot spots) are recorded corresponding to the combustion cells observed in Fig. 8c, 8d, 10c. Fig. 14. RGB hyperspectral image of the combustion of a mixture of 40% H2 - air, initiated by a platinum wire, obtained using a modified VID-IK3 hyperspectrometer, T0 = 320 0C, P0 = 1 atm, spectral interval 550 - 650 nm. The main feature of these “hot spots” is that the emission spectra of combustion along and across these points, depending on both the y coordinate and x (time), behave unsympathetically and have a maximum inside this point. Fig. 15. Dependence of the intensity of combustion emission spectra for different values of x (along the red line in Fig. 2a) for point 1 (Fig. 14). The spectra along one of these points (point 1 in Fig. 14) for different values of x (along the red line in Fig. 2a) is shown in fig. 15. The dependence of the position of the spectrum maximum for a wavelength of 972 nm on the x coordinate for point 1 (Fig. 14) is demonstrated in fig. 16. Fig. 16. Dependence of the position of the spectrum maximum for a wavelength of 972 nm on the x coordinate for point 1 (Fig. 14). The spectra across point 1 for different values of y (time) is indicated in fig. 17. Fig. 17. Dependence of the emission spectra of combustion on y (time) for point 1 (Fig. 14) The dependence of the intensity maximum for the 972 nm line (Fig. 18) of point 1 (Fig. 14) on y (time) is shown in fig. 18 . Fig. 18. Dependence of the maximum intensity for the line 972 nm (Fig. 16) point 1 (Fig. 14) on y (time) As seen from Fig. 16 and 18, the spectral intensities for these points do not behave symbatically. It is interesting to note that these points are displaced along the x-axis depending on the recording time, that is, as cells that change their position in the video frames in Fig. 8c, 8d, 10c. An important conclusion also follows from the data obtained that the emission spectrum of the cells is close to the emission spectrum of a gray body (intensity maxima in space are observed simultaneously in different parts of the investigated spectral interval), that is, the emission of points (cells) really corresponds to the glow of incandescent catalyst particles. Let us stop on the features of the emission spectrum of hydrogen combustion in a heated reactor in the presence of a platinum wire. It can be seen from fig. 12a (compare also with Figs 4d and 12b) that in this case an additional band at 552 nm appears in the emission spectrum of the hydrogen flame. According to the literature, the nature of the appearance of radiation at this wavelength has not yet been established. The indicated band in the emission spectrum (Fig.13a) is observed during intense combustion of rich mixtures of industrial hydrocarbons, i.e. in the presence of soot particles [20], as well as in the combustion of methane in the presence of heated coal dust. Obviously, in both of these cases, neither hydrogen nor platinum is involved in the combustion process. Therefore, for this study, to find out whether the radiation source at a wavelength of 552 nm is associated with the evaporation of platinum oxide from a heated platinum surface was of fundamental importance. For this purpose, a cylindrical furnace 6 cm in diameter and 3 cm long was placed in reactor 1. minutes to 400 0C and a stoichiometric mixture of natural gas with oxygen up to 150 mm Hg was admitted in installation 2 (Fig. 2). Ignition was initiated by a spark discharge. The emission spectrum recorded using optical spectroscopy is shown in Fig. 19a. As seen from Fig. 19a, the 552 nm band is clearly observed in this spectrum. However, as indicated above, to observe this band, a hydrocarbon is needed as a combustible, as well as a heated coal powder. In the next experiment, the conditions remained the same, only methane was replaced by hydrogen. At the same time, the 552 nm band remained in the spectrum. In the absence of carbon dust in a clean (washed with ethanol) reactor, this band was no longer observed (cf. Figs. 4d and 12b) both upon initiation of ignition by a spark discharge or by a heated platinum wire. Thus, the method of initiating the ignition is not associated with the occurrence of this emission band. This led us to the conclusion that experiments at room temperature and in a heated reactor differ methodically by the presence of an aluminum ring to prevent gas circulation in the heated reactor (see Experimental part). Therefore, a thin aluminum foil was introduced into the “cold” reactor, which was used to cover the inner walls of the reactor. The initiation was carried out with a heated platinum wire. The result of the experiment is shown in Fig. 19b, and the result of its digital processing using the Hesperus 3.0 program is shown in Fig. 19c. It can be seen from fig. 19b that when a mixture of 40% H2 - air is ignited, it is possible to observe a band at 552 nm. It should be noted that the appearance of copper lines (515, 521, 529, 532 nm [21]) is because the platinum wire was attached to copper electrodes, which were heated at the attachment points. Thus, the occurrence of emission at a wavelength of 552 nm is most likely due to the radiation of metal impurities contained in aluminum. Excitation of metal atoms is carried out during the recombination of atoms and radicals arising during combustion on the hot surface of aluminum (the flame temperature of a mixture of 40% H2 - air is ~ 2200 0С [22]) with the release of a significant amount of energy. For example, it is known that a platinum wire placed at a distance of 7 cm from an RF discharge can even melt due to the energy released during the recombination of oxygen atoms on the surface (2O → O2 + 116.4 kcal/mol) [23]. Fig. 19. a) - optical spectrum of radiation during combustion of a stoichiometric mixture of methane in oxygen in the presence of carbon dust heated to 400 °C. P = 150 mm Hg; b) - optical spectrum of hydrogen combustion in air upon initiation by a heated platinum wire in the presence of a thin (0.1 mm) aluminum foil covering the reactor walls. P = 1 atm, initial temperature 20 ° C. c) - spectrum b after processing using the Hesperus 3.0 software package. This energy corresponds to ultraviolet radiation at a wavelength of about 270 nm. Sources of radiation at a wavelength of 552 nm can be impurities of atoms of alkaline earth metals in industrial aluminum, which contains Fe, Cu, Mn, Mg, Cr, Ni [24] and trace amounts of alkali and alkaline earth metals, in particular, Ca [25]. As shown in [26], excited CaOH and CuOH (calcium monohydroxide, copper monohydroxide) molecules can provide radiation at 552 nm. Since carbon powders contain a large amount of inorganic impurities, including metals and their salts [27], the 552 nm band during coal combustion is obviously of the same origin. This result also means that the introduction of platinum into the hydrogen oxidation flame does not lead to changes in the visible emission spectrum of this flame as compared to initiation by an electric discharge. Thus, the processes of evaporation and decomposition of Pt oxide, which has catalytic properties, like platinum itself, determine the role of platinum. Directly related to these processes is the cellular mode discovered in this work for the Pt-initiated combustion of a mixture of 40% H2 with air - a composition close to stoichiometric. Thus, in accordance with the above, during the ignition delay period in the gas phase, molecules or clusters of Pt and platinum oxide are formed at the temperature of the platinum wire in the combustible gas above 500 0C. Pt-containing ultrafine particles diffusing into the reaction volume act as catalytic centers on which hydrogen is oxidized, which leads to strong heating of these particles. These incandescent particles are perceived as flame cells on video filming and when recording by the 4D spectroscopy method. In fact, they are such cells in the area of which combustion occurs most intensely. We point out that the rate of diffusion of catalytic particles in the gas should determine the possibility of implementing cellular combustion. This is indeed the case. For example, the diffusion rate of catalytic particles decreases in the presence of 15% CO2. These particles “do not keep up” behind the propagating combustion front (Fig. 8d), and the cellular combustion mode is not recorded. On the other hand, the addition of 15% light He (Fig. 8e) does not lead to the disappearance of the cellular combustion regime. Let us turn to the analysis of the temperature dependences of the ignition delay times during the combustion of hydrogen in the presence of a platinum surface in a heated reactor. The ignition delay time  is one of the most important macrokinetic characteristics of thermal ignition, which can be measured in relatively simple ways. In this case, an important experimental fact is that, according to [26, 28], in a shock tube and in a rapid compression machine, thermal ignition has a cellular nature. We have also recently shown [3, 7] that the ignition of mixtures of hydrogen and n-pentane with air in a bypass plant at a total pressure of 0.6 - 2 atm begins with the appearance of a primary focus on the most chemically active area of the surface (see paragraph 4 of Chapter 3). Thus, thermal ignition includes the stages of warm-up, focal ignition and flame propagation. This means that cellular ignition is the rule, not the exception, i.e. “self-ignition” as a process that occurs simultaneously in the entire volume of the reactor, apparently, is not provided in principle. The temperature dependence of the ignition delay times for a mixture of 40% H2 and air in the reactor in the presence and in the absence of a gas flow (Fig. 19) above the catalytic surface (Pt foil or Pt wire) in Arrhenius coordinates is shown in fig. 20. As seen from Fig. 20, the effective activation energy E is practically the same for both the Pt foil and the Pt wire, both in the presence and in the absence of a gas flow. The experimental value of E is 19 ± 3 kcal/mol and is close to the rate constant of the hydrogen combustion branching reaction H + O2 → OH + O (16.7 kcal/mol [22, 29]). This means that the ignition delay in the initiation of hydrogen combustion by the platinum surface is determined by the slowest stage of the kinetic mechanism, namely, the branching reaction, the slowest stage in the sequence of reactions leading to flame propagation. Indeed, the value of the delay period for the initial stage of the combustion process is  ≈ 1/, where  is the so-called branching factor, which includes the value of the rate constant of the activated branching reaction in the case of a hydrogen oxidation reaction. As is known [22], the coordinate of the point of intersection of straight lines with the ordinate axis in Fig. 20 is approximately inversely proportional to the frequency of active collisions. Since the surface area of the Pt wire is less than that of the Pt foil, the frequency of collisions with the surface is lower for the Pt wire. In addition, the collision frequency for a Pt foil in a stationary gas is less than for the same foil in a circulating gas. This is illustrated in Fig. 20. Conclusions for Chapter 5 A cellular mode of combustion of a 40% hydrogen - air mixture in the presence of platinum wire and foil in the range of 270-350 0C at atmospheric pressure was discovered. Time and coordinate, and high-speed color filming, combustion cells caused by catalytic instability have been experimentally detected for the first time using the 4D optical spectroscopy method, which allows recording the intensity of the optical spectrum simultaneously depending on the wavelength. Fig. 20. Temperature dependence of the delay times of thermal ignition for a mixture of 40% H2 with air in the reactor of the bypass plant in the presence and in the absence of a gas flow at a pressure of 1 atm. Black triangles - ignition initiated by platinum foil, gas at rest; black squares - platinum foil initiated ignition, circulating gas; empty squares - ignition initiated by platinum wire, gas at rest. It was found that the cellular mode is determined by the catalytic combustion of hydrogen on Pt - containing particles formed during the decomposition of unstable platinum oxide in the gas phase. During the ignition delay period at the temperature of the platinum wire in the combustible gas above 5000 0C, molecules or clusters of Pt oxide and platinum are formed in the gas phase. Pt-containing ultrafine particles diffusing into the reaction volume act as catalytic centers on which hydrogen is oxidized, which leads to strong heating of these particles. These incandescent particles are perceived as flame cells on video filming and, in fact, are such cells in the area of which combustion is most intense. It is shown that the temperature dependence of the hydrogen ignition delays on a platinum wire and foil in both stationary and rotating gases corresponds to an activation energy of 19 ± 3 kcal/mol, which is close to the activation energy of branching of hydrogen oxidation reaction chains. The impurity origin of the 552 nm emitting band, which is often recorded during combustion of gas and dust-gas mixtures, has been established. The results obtained are of immediate importance for the development of Catalytic Stabilization (CS) technology and the development of catalysts with increased activity. The results are also important for verification of theoretical concepts of the propagation of dust and gas flames.

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