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1.
The effect of CO addition on extinction and NO x formation in lean premixed counterflow CH4/air flames was investigated by numerical simulation. Detailed chemistry and complex thermal and transport properties were employed. A method that gradually switched off the initial reactions of NO formation from different routes was used to analyse the variation of NO formation mechanism. The results indicate that the addition of certain amount of CO increases the strain extinction limits and reduces the radiation extinction limits. As a result, the lean flammability limit of CH4/air premixed flame is extended to leaner side by the addition of CO. The formation of NO in a flame is increased with the addition of CO at a constant equivalence ratio. For an ultra-lean flame, the increase in the formation of NO is mainly because of the increase in the contribution from the NNH intermediate route, while for a near stoichiometric flame, this increase is mainly attributable to the rise in the contribution from the thermal route. With the fraction of added CO being gradually increased, the formation of NO2 in a flame first decreases and then increases at a given equivalence ratio. The addition of CO reduces the formation N2O in an ultra-lean flame, while affects little on the formation of N2O in a near stoichiometric flame.  相似文献   

2.
We investigate the effects of varying the degree of burner stabilization on Fenimore NO formation in fuel-rich low-pressure flat CH4/O2/N2 flames. Towards this end, axial profiles of flame temperature and OH, NO and CH mole fractions are measured using laser-induced fluorescence (LIF). The experiments are performed at equivalence ratios between 1.3 and 1.5. The flame temperature is seen to decrease by 200-300 K, with a concomitant decrease in OH mole fraction, upon reducing the total flow rate from 5 to 3 L/min, thus increasing stabilization. At equivalence ratios between 1.3 and 1.5, this decrease in flow rate lowers the maximum CH mole fraction by a factor of 2, and the NO mole fraction by ∼40% in all flames studied. Integrating the reaction rate for CH + N2 to estimate Fenimore NO formation, using the rate coefficient in GRI-Mech 3.0, and the measured temperatures and CH profiles show very good agreement with the measured NO mole fraction for ? = 1.3 and 1.4, supporting the current choice for this rate. This agreement also shows that the increase in residence time caused by increased stabilization is an important factor in the ultimate impact of the changes in CH mole fraction on NO formation. The results at ? = 1.5 suggest that substantial quantities of fixed nitrogen species, e.g., HCN, are only slowly oxidized in the post-flame zone under these conditions, leading to a significant discrepancy between the measured NO mole fraction and that obtained by integrating over the CH profile. Detailed calculations using GRI-Mech 3.0 predict the experimental results at ? = 1.3 nearly quantitatively, but show increasing differences with the measurements for both CH and NO profiles with increasing equivalence ratio.  相似文献   

3.
In order to achieve carbon neutrality, the use of ammonia as a fuel for power generation is highly anticipated. The utilization of a binary fuel consisting of ammonia and hydrogen can address the weak flame characteristics of ammonia. In this study, the product gas characteristics of ammonia/hydrogen/air premixed laminar flames stabilized in a stagnation flow were experimentally and numerically investigated for various equivalence ratios for the first time. A trade-off relationship between NO and unburnt ammonia was observed at slightly rich conditions. At lean conditions, NO reached a maximum value of 8,700 ppm, which was larger than that of pure ammonia/air flames. The mole fraction of nitrous oxide (N2O) which has large global warming potential rapidly increased around the equivalence ratio of 0.6, which was attributed to the effect of a decrease in flame temperature downstream of the reaction zone owing to heat loss to the stagnation wall. To understand this effect further, numerical simulations of ammonia/hydrogen/air flames were conducted using the stagnation flame model for various equivalence ratios and stagnation wall temperatures. The results show that the important reactions for N2O production and reductions are NH +NO = N2O + H, N2O + H = N2 + OH, and N2O (+M) = N2 + O (+M). A decrease in flame temperature in the post flame region inhibited N2O reduction through N2O (+M) = N2 + O (+M) because this reaction has a large temperature dependence, and thus N2O was detected as a product gas. N2O is reduced through N2O (+M) = N2 + O (+M) in the post flame region if the stagnation wall temperature is sufficiently high. On the other hand, it was clarified that an increase in equivalence ratio enhances H radical production and promotes N2O reduction by H radical through the reaction of N2O + H = N2 + OH.  相似文献   

4.
An experimental study on CH4–CO2–air flames at various pressures is conducted by using both laminar and turbulent Bunsen flame configurations. The aim of this research is to contribute to the characterization of fuel lean methane/carbon dioxide/air premixed laminar and turbulent flames at different pressures, by studying laminar and turbulent flame propagation velocities, the flame surface density and the instantaneous flame front wrinkling parameters. PREMIX computations and experimental results indicate a decrease of the laminar flame propagation velocities with increasing CO2 dilution rate. Instantaneous flame images are obtained by Mie scattering tomography. The image analysis shows that although the height of the turbulent flame increases with the CO2 addition rate, the flame structure is quite similar. This implies that the flame wrinkling parameters and flame surface density are indifferent to the CO2 addition. However, the pressure increase has a drastic effect on both parameters. This is also confirmed by a fractal analysis of instantaneous images. It is also observed that the combustion intensity ST/SL increases both with pressure and the CO2 rate. Finally, the mean fuel consumption rate decreases with the CO2 addition rate but increases with the pressure.  相似文献   

5.
NOx formation was measured during combustion of pulverized coals and pulverized coal char in N2 and CO2 environments under isothermal and nearly constant oxygen conditions (i.e. using dilute coal loading). Three different oxygen concentrations (12% O2, 24% O2, and 36% O2) and two representative US coals were investigated, at a gas temperature of 1050 °C. To investigate the importance of NO reburn reactions, experiments were also performed with an elevated concentration (550 ppm) of NO in the gases into which the coal was introduced. For low levels of background NO, the fractional fuel-nitrogen conversion to NOx increases dramatically with increasing bath gas oxygen content, for both N2 and CO2 environments, though the fuel conversion is generally lower in CO2 environments. Char N conversion is lower than volatile N conversion, especially for elevated O2 concentrations. These results highlight the importance of the volatile flame and char combustion temperatures on NOx formation. For the high background NOx condition, net NOx production is only observed in the 36% O2 environment. Under these dilute loading conditions, NO reburn is found to be between 20% and 40%, depending on the type of coal, the use of N2 or CO2 diluent, the bulk O2 concentration, and whether or not one considers reburn of volatile-NOx. This dataset provides a unique opportunity to understand and differentiate the different sources and sinks of NOx under oxy-fuel combustion conditions.  相似文献   

6.
Chemical energy vectors will play a crucial role in the transition of the global energy system, due to their essential advantages in storing energy in form of gaseous, liquid, or solid fuels. Ammonia (NH3) has been identified as a highly promising candidate, as it is carbon-free, can be stored at moderate pressures, and already has a developed distribution infrastructure. As a fuel NH3 has poor combustion properties that can be improved by the addition of hydrogen, which can be obtained energy-efficiently by partially cracking ammonia into hydrogen (H2) and nitrogen (N2) prior to the combustion process. The resulting NH3/H2/N2 blend leads to significantly improved flame stability and resilience to strain-induced blow-out, despite similar laminar flame properties compared to equivalent methane/air flames. This study reports the first measurements of extinction strain rates, measured using the premixed twin-flame configuration in a laminar opposed jet burner, for two NH3/H2/N2 blends over a range of equivalence ratios. Local strain rates are measured using particle tracking velocimetry (PTV) and are related to the inflow conditions, such that the local strain rate at the extinction point can be approximated. The results are compared with 1D-simulations using three recent kinetic mechanisms for ammonia oxidation. By relating the extinction strain rates to laminar flame properties of the unstretched flame, a comparison of the extinction behaviour of CH4 and NH3/H2/N2 blends can be made. For lean mixtures, NH3/H2/N2-air flames show a significant higher extinction resistance in comparison to CH4/air. In addition, a strong non-linear dependence between the resistance to extinction and equivalence ratio for NH3/H2/N2 blends is observed.  相似文献   

7.
The chemistry of char-N release and conversion to nitrogen-containing products has been probed by studying its release and reactions with O2, CO2, and H2O. The experiments were performed in a fixed bed flow reactor at pressures of up to 1.0 MPa. The results show that the major nitrogen-containing products observed depend on the reactant gas; with O2, NO, and N2 being the major species observed. Char-N reaction with CO2 produces N2 with very high selectivity over a broad range of pressures and CO2 concentrations, and reaction with H2O gives rise to HCN, NH3, and N2. Observed distributions of nitrogen-containing products are little affected by pressure when O2 and CO2 are the reactant gases, but increasing pressures in the reaction with H2O results in the formation of increasing proportions of NH3. Formation of NH3 is also promoted by increasing concentrations of H2O in the feed gas. The results suggest that NO and HCN are primary products when O2 and H2O, respectively, are used as the reactant gases, and that the other observed products arise from interactions of these primary products with the char surface.  相似文献   

8.
In this study, a bespoke single-stage swirl burner was used to experimentally investigate the effects of residence time on emissions from premixed ammonia-methane-air flames. The residence time was altered in two ways: by modifying the combustion chamber's length or by modifying the swirl number. Exhaust emissions of O2, CO2, CO, NO, NO2, and N2O were measured at an absolute pressure of 2 bar for equivalence ratios between 0.50 and 0.95 and ammonia fractions in the fuel blend between 0 and 100%. Spatial distributions of NO and OH radicals were also imaged using PLIF inside the combustion chamber at different heights above the nozzle. Data shows that increasing residence time can further advance chemical reactions, as evidenced by a reduction in O2 concentration in the exhaust. Increasing the swirl number reduces emissions of NO, NO2, and N2O more efficiently than tripling the chamber's length. However, a decrease in the combustion efficiency may be responsible for a fraction of this NOx reduction when the swirl number is increased for some equivalence ratios. NO emissions are not modified when the chamber's length is increased, which is consistent with the fact that the NO-LIF signal does not decay when the distance from the nozzle increases. Therefore, NO formation is somehow restricted to within the main reaction zone of the swirling flame, that is, the zone whose height does not exceed 60 mm for this burner. Conversely, tripling the chamber's length reduces the concentrations of NO2 and N2O. This reduction is not reflected in a measurable increase in NO concentration because NO is present in much larger quantities than NO2 and N2O in flames examined here. Consistent with the fact that OH promotes NO formation via fuel-NOx pathways, a positive correlation is found between NO- and OH-LIF intensities.  相似文献   

9.
This paper reported the analysis of dilution effects on the opposed-jet H2/CO syngas diffusion flames. A computational model, OPPDIF coupled with narrowband radiation calculation, was used to study one-dimensional counterflow syngas diffusion flames with fuel side dilution from CO2, H2O and N2. To distinguish the contributing effects from inert, thermal/diffusion, chemical, and radiation effects, five artificial and chemically inert species XH2, XCO, XCO2, XH2O and XN2 with the same physical properties as their counterparts were assumed. By comparing the realistic and hypothetical flames, the individual dilution effects on the syngas flames were revealed. Results show, for equal-molar syngas (H2/CO = 1) at strain rate of 10 s?1, the maximum flame temperature decreases the most by CO2 dilution, followed by H2O and N2. The inert effect, which reduces the chemical reaction rates by behaving as the inert part of mixtures, drops flame temperature the most. The thermal/diffusion effect of N2 and the chemical effect of H2O actually contribute the increase of flame temperature. However, the chemical effect of CO2 and the radiation effect always decreases flame temperature. For flame extinction by adding diluents, CO2 dilution favours flame extinction from all contributing effects, while thermal/diffusion effects of H2O and N2 extend the flammability. Therefore, extinction dilution percentage is the least for CO2. The dilution effects on chemical kinetics are also examined. Due to the inert effect, the reaction rate of R84 (OH+H2 = H+H2O) is decreasing greatly with increasing dilution percentage while R99 (CO+OH→CO2+H) is less affected. When the diluents participate chemically, reaction R99 is promoted and R84 is inhibited with H2O addition, but the trend reverses with CO2 dilution. Besides, the main chain-branching reaction of R38 (H+O2→O+OH) is enhanced by the chemical effect of H2O dilution, but suppressed by CO2 dilution. Relatively, the influences of thermal/diffusion and radiation effects on the reaction kinetics are then small.  相似文献   

10.
利用密度泛函理论通过计算吸附能量、HOMO/LUMO能隙变化、电荷转移、结构扭曲等研究二氧化氮分子在B12N12纳米笼的吸附.此外,通过计算B12N12的电子结合能、Gibbs自由能、态密度和分子表面的静电势研究其稳定性和其它特性.B12N12纳米笼吸附二氧化氮显示三种构型.B12N12团簇的HOMO/LUMO能隙变化对二氧化氮分子的存在非常敏感,从自由团簇的6.84 eV降为NO2/团簇稳定团簇的3.23 eV.团簇的导电性被极大地提高,表明B12N12纳米簇可能是潜在的二氧化氮气体分子检测传感器.  相似文献   

11.
Structures of several premixed ethylene-oxygen-argon rich flat flames burning at 50 mbar have been established by using molecular beam mass spectrometry in order to investigate the effect of CO2, or NH3, or H2O addition on species concentration profiles. The aim of this study is to examine the eventual changes of profiles of detected hydrocarbon intermediates which could be considered as soot precursors (C2H2, C4H2, C5H4, C5H6, C6H2, C6H4, C6H6, C7H8, C6H6O, C8H6, C8H8, C9H8 and C10H8). The comparative study has been achieved on four flames with an equivalence ratio (f) of 2.50: one without any additive (F2.50), one with 15% of CO2 replacing the same quantity of argon (F2.50C), one with 3.3% of NH3 in partial replacement of argon (F2.50N) and one with 13% of H2O in replacement of the same quantity of argon (F2.50H). The four flat flames have similar final flame temperatures (1800 K).CO2, or NH3, or H2O addition to the fresh gas inlet causes a shift downstream of the flame front and thus flame inhibition. Endothermic processes CO2 + H = CO + OH and H2O + H = H2 + OH are responsible of the reduction of the hydrocarbon intermediates in the CO2 and H2O added flames through the supplementary formation of hydroxyl radicals. It has been demonstrated that such processes begin to play at the end of the flame front and becomes more efficient in the burnt gases region.The replacement of some Ar by NH3 is responsible only for a slight decrease of the maximum mole fraction of C2H2, but NH3 becomes much more efficient for C4H2 and C5 to C10 species. Moreover, the efficiency of NH3 as a reducing agent of C5 to C10 intermediates is larger than that of CO2 and H2O for equal quantities added.  相似文献   

12.
Experimental measurements of the adiabatic burning velocity in neat and NO formation in CH4 + O2 + Ar flames doped with small amounts of N2O are presented. The oxygen content in the oxidizer was varied from 15 to 17%. Non-stretched flames were stabilized on a perforated plate burner at 1 atm. The Heat Flux method was used to determine burning velocities under conditions when the net heat loss of the flame is zero. Adiabatic burning velocities of methane + oxygen + argon mixtures were found in satisfactory agreement with the modeling. The NO concentrations in the flames doped with N2O (100 ppm in the argon stream before mixing) were measured in the burnt gases at a fixed distance from the burner using probe sampling. Axial profiles of [NO] were found insensitive to the downstream heat losses. Experimental dependencies of [NO] versus equivalence ratio had a maximum between φ = 1.1 and 1.2. Calculated concentrations of NO were in good agreement with the measurements. In lean flames calculated concentrations of NO strongly depends on the rate constant of reaction N2O + O=NO + NO if too high values proposed in the literature are employed. These new experimental data thus allowed for validation of the key reactions of the nitrous oxide mechanism of NO formation in flames.  相似文献   

13.
The effects of NO and NO2 produced by using a plasma jet (PJ) of a N2/O2 mixture on ignition of hydrogen, methane, and ethylene in a supersonic airflow were experimentally and numerically investigated. Numerical analysis of ignition delay time showed that the addition of a small amount of NO or NO2 drastically reduced ignition delay times of hydrogen and hydrocarbon fuels at a relatively low initial temperature. In particular, NO and NO2 were more effective than O radicals for ignition of a CH4/air mixture at 1200 K or lower. These ignition enhancement effects were examined by including the low temperature chemistry. Ignition tests by a N2/O2 PJ in a supersonic flow (M = 1.7) for using hydrogen, methane, and ethylene injected downstream of the PJ were conducted. The results showed that the ignitability of the N2/O2 PJ is affected by the composition of the feedstock and that pure O2 is not the optimum condition for downstream fuel injection. This result of ignition tests with downstream fuel injection demonstrated a significant difference in ignition characteristics of the PJ from the ignition tests with upstream fuel injection.  相似文献   

14.
The kinetic effects of NO addition on the flame dynamics and burning limits of n-dodecane cool and warm diffusion flames are investigated experimentally and computationally using a counterflow system. The results show that NO plays different roles in cool and warm flames due to their different reaction pathway sensitivities to the flame temperature and interactions with NO. We observe that NO addition decreases the cool flame extinction limit, delays the extinction transition from warm flame to cool flame, and promotes the ignition transition from warm flame to hot flame. In addition, jet-stirred reactor (JSR) experiments of n-dodecane oxidation with and without NO addition are also performed to develop and validate a n-dodecane/NOx kinetic model. Reaction pathway and sensitivity analyses reveal that, for cool flames, NO addition inhibits the low-temperature oxidation of n-dodecane and reduces the flame temperature due to the consumption of RO2 via NO+RO2?NO2+RO, which competes with the isomerization reaction that continues the peroxy radical branching sequence. The model prediction captures well the experimental trend of the inhibiting effect of NO on the cool flame extinction limit. For warm flames, two different kinds of warm flame transitions, the warm flame extinction transition to cool flame and the warm flame reignition transition to hot flame, were observed. The results suggest that warm extinction transition to cool flame is suppressed by NO addition while the warm flame reignition transition to hot flame is promoted. The kinetic model developed captures well the experimentally observed warm flame transitions to cool flame but fails to predict the warm flame reignition to hot flame at similar experimental conditions.  相似文献   

15.
The role of methylene in prompt NO formation   总被引:1,自引:0,他引:1  
We address the plausibility of singlet methylene (1CH2) in the prompt NO formation mechanism via examination of experimental species profiles and kinetic flame modeling of several low-pressure methane-oxygen-nitrogen flames. Existing kinetic models assuming CH as the only prompt NO precursor greatly underpredict NO formation under very fuel-lean conditions. We have constructed a kinetic pathway initiated by the recombination of singlet CH2 with molecular nitrogen to form diazomethane, CH2NN, early in the flame. Although the majority of the diazomethane is predicted to react with flame radicals to regenerate N2, a small percentage (approximately 10%) is predicted to react via cleavage of the NN bond leading to NO formation. This leads to accurate prediction of the experimental measurements of NO formation in lean, low-pressure flames. Assuming reasonable kinetic parameters for the reactions of CH2, the large underprediction of NO under lean conditions can be rectified by the inclusion of the 1CH2 prompt NO pathway in the kinetic mechanism.  相似文献   

16.
Yuhai Hu  Keith Griffiths   《Surface science》2009,603(17):2835-2840
NO dissociation and subsequent N2 production in the presence of co-adsorbed S18O2 and D2 on the surface of stepped Pt(3 3 2) were studied using Fourier transform infra red reflection–absorption spectroscopy (FTIR-RAS) combined with thermal desorption spectroscopy (TDS). Reduction of NO by D (D2 is adsorbed dissociatively on Pt surfaces) proceeds to a limited extent, because this reaction is rate-controlled by NO dissociation and the supply of D atoms at the higher surface temperatures at which NO dissociation becomes significant (350 K and higher). NO–D reaction is suppressed in the presence of S18O2, depending significantly on the S18O2 coverage and the competition between the reactions NO–D and S18O2–D. When the supply of D2 is limited, e.g., 0.1 L in this study, the presence of S18O2 suppresses the NO–D reaction. With a sufficient supply of D2, e.g., 0.4 L and higher, D-atom competing reactions do not play a role any more because the reactions of both NO and S18O2 with D proceed only to a very limited extent. As such, generation of O atoms from S18O2 dissociation is the main reaction that leads to the suppression in NO dissociation and consequently, N2 production.It is also concluded that the presence of S18O2 does not seriously poison the active sites on the Pt surface, providing that there is a sufficient D supply to remove O atoms from both NO dissociation and S18O2 dissociation.  相似文献   

17.
We present experimental results from turbulent low-swirl lean H2/CH4 flames impinging on an inclined, cooled iso-thermal wall, based on simultaneous stereo-PIV and OH×CH2O PLIF measurements. By increasing the H2 fraction in the fuel while keeping Karlovitz number (Ka) fixed in a first series of flames, a fuel dependent near-wall flame structure is identified. Although Ka is constant, flames with high H2 fraction exhibit significantly more broken reaction zones. In addition, these high H2 fraction flames interact significantly more with the wall, stabilizing through the inner shear layer and well inside the near-wall swirling flow due to a higher resistance to mean strain rate. This flame-wall interaction is argued to increase the effective local Ka due to heat loss to the wall, as similar flames with a (near adiabatic) ceramic wall instead of a cooled wall exhibit significantly less flame brokenness. A second series of leaner flames were investigated near blow-off limit and showed complete quenching in the inner shear layer, where the mean strain rate matches the extinction strain rate extracted from 1D flames. For pure CH4 flames (Ka ≈ 30), the reaction zone remains thin up to the quenching point, while conversely for the 70% H2 flames (Ka ≈ 1100), the reaction zone is highly fragmented. Remarkably, in all near blow-off cases with CH4 in the fuel, a large cloud of CH2O persists downstream the quenching point, suggesting incomplete combustion. Finally, ultra lean pure hydrogen flames were also studied for equivalence ratios as low as 0.22, and through OH imaging, exhibit a clear transition from a cellular flame structure to a highly fragmented flame structure near blow-off.  相似文献   

18.
The influence of wall heat loss on the emission characteristics of ammonia-air swirling flames has been investigated employing Planar Laser-Induced Fluorescence imaging of OH radicals and Fourier Transform Infrared spectrometry of the exhaust gases in combustors with insulated and uninsulated walls over a range of equivalence ratios, ?, and pressures up to 0.5 MPa. Strong influence of wall heat loss on the flames led to quenching of the flame front near the combustor wall at 0.1 MPa, resulting in large unburned NH3 emissions, and inhibited the stabilization of flames in the outer recirculating zone (ORZ). A decrease in heat loss effects with an increase in pressure promoted extension of the fuel-rich stabilization limit owing to increased recirculation of H2 from NH3 decomposition in the ORZ. The influence of wall heat loss resulted in emission trends that contradict already reported trends in literature. NO emissions were found to be substantially low while unburned NH3 and N2O emissions were high at fuel-lean conditions during single-stage combustion, with values such as 55 ppmv of NO, 580 ppmv of N2O and 4457 ppmv of NH3 at ? = 0.8. In addition, the response of the flame to wall heat loss as pressure increased was more important than the effects of pressure on fuel-NO emission, thereby leading to an increase in NO emission with pressure. It was found that a reduction in wall heat loss or a sufficiently long fluid residence time in the primary combustion zone is necessary for efficient control of NH3 and N2O emissions in two-stage rich-lean ammonia combustors, the latter being more effective for N2O in addition to NO control. This study demonstrates that the influence of wall heat loss should not be ignored in emissions measurements in NH3-air combustion, and also advances the understanding of previous studies on ammonia micro gas turbines.  相似文献   

19.
Experiments were conducted on a laminar premixed ethylene-air flame at equivalence ratios of 2.34 and 2.64. Comparisons were made between flames with 5% NO2 added by volume. Soot volume fraction was measured using light extinction and light scattering and fluorescence measurements were also obtained to provide added insight into the soot formation process. The flame temperature profiles in these flames were measured using a spectral line reversal technique in the non-sooting region, while two-color pyrometry was used in the sooting region. Chemical kinetics modeling using the PREMIX 1-D laminar flame code was used to understand the chemical role of the NO2 in the soot formation process. The modeling used kinetic mechanisms available in the literature. Experimental results indicated a reduction in the soot volume fraction in the flame with NO2 added and a delay in the onset of soot as a function of height above the burner. In addition, fluorescence signals—often argued to be an indicator of PAH—were observed to be lower near the burner surface for the flames with NO2 added as compared to the baseline flames. These trends were captured using a chemical kinetics model that was used to simulate the flame prior to soot inception. The reduction in soot is attributed to a decrease in the H-atom concentration induced by the reaction with NO2 and a subsequent reduction in acetylene in the pre-soot inception region.  相似文献   

20.
Yuhai Hu  Keith Griffiths   《Surface science》2008,602(17):2949-2954
Fourier transform infra red reflection–absorption spectroscopy (FTIR-RAS), thermal desorption spectroscopy (TDS), and auger electron spectroscopy (AES), were employed to explore the mechanism of NO reduction in the presence of C2H4 on the surface of stepped Pt(3 3 2). Both NO–Pt and C2H4–Pt interactions are enhanced when NO and C2H4 are co-adsorbed on Pt(3 3 2). As a result, C2H4 is dissociated at surface temperatures as low as 150 K, and the N–O stretch band is weakened. The presence of post-exposed C2H4 leads NO desorption from steps to decrease significantly, but the same effect on NO desorption from terraces becomes appreciable only at higher post-exposures of C2H4, e.g., 0.6 L and 1.2 L, and proceeds to a much slighter extent. Auger spectra indicate that as a result of the reaction with O from NO dissociation, the amount of surface C species is greatly reduced when NO is post-exposed to a C2H4 adlayer. It is concluded that reduction of NO in the presence of C2H4 proceeds very effectively on the surface of the Pt(3 3 2), through a mechanism of NO dissociation and subsequent O removal. Following this mechanism, the significant dissociation of adsorbed NO molecules on steps at surface temperatures below 400 K, and subsequent rapid reaction between the resultant O and C-related species, accounts for the considerable amount of N2 desorption at temperatures below 400 K.  相似文献   

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