Spectral radiation characterization of OH*, NH2* and NH* in ammonia/methane diffusion flame

doi:10.11949/0438-1157.20230989

Abstract

Abstract:

Based on the flame spectroscopy diagnostic platform, a spectral imaging system was utilized to obtain the OH*, NH₂* and NH* radiation distributions of the ammonia/methane diffusion flame. The reaction mechanism was explored in the CHEMKIN. The results show that compared with pure methane combustion, the OH* radiation distribution zone and radiation intensity of the flame after ammonia blending are significantly reduced, and the distribution pattern extends outwards downstream of the flame. With the increase of ammonia blending ratio, the radiation distribution zone of NH₂* was raised to the downstream of the flame, and the radiation intensity increased. NH* radiation distribution zone was basically unchanged. The radiation intensity of NH* increased and then decreased with the increase of ammonia blending ratio. NH* radiation intensity reached the maximum when the ammonia fraction was from 0.2 to 0.3. The radiative intensity of the three radicals increased with the equivalence ratios, in which the distribution of OH* was biased toward the oxidant side, while NH₂* and NH* were biased toward the fuel side. With the addition of NH₂* and NH* reaction mechanisms, the simulation show that the main source of NH₂* was the dehydrogenation process of ammonia. The changes in the ammonia blending ratio directly affected the generation of NH₂*. The maximum production reaction of NH* indicated that the rate of the reaction generation of NH* was affected by the mixing ratio of ammonia and methane.

Key words: ammonia, methane, diffused, radicals, spectral radiation

摘要：

基于火焰光谱诊断平台，利用光谱成像系统获得氨/甲烷扩散火焰的OH*、NH₂*和NH*辐射分布，并结合CHEMKIN探究其反应机理。结果表明：与纯甲烷燃烧相比，氨掺混后火焰的OH*辐射分布区域和辐射强度均降低较明显，在火焰下游分布形态向外延展。随着氨掺混比例的增加，NH₂*辐射分布区域向火焰下游拉升，辐射强度增加。NH*辐射分布区域基本不变，辐射强度随氨掺混比例的增加先增加后降低，在氨分数为0.2~0.3时达到最大。三个自由基辐射强度均随当量比增大而增加，其中OH*分布偏向氧化剂侧，NH₂*和NH*偏向燃料侧。添加NH₂*和NH*反应机理后，模拟结果显示，NH₂*的主要来源为氨的脱氢过程，掺氨比例的变化直接影响NH₂*的生成，NH*最大生成反应的反应生成率受氨和甲烷混合比例的影响。

关键词: 氨, 甲烷, 扩散, 自由基, 光谱辐射

CLC Number:

O 433.52

Zhengqiao DUAN, Yan GONG, Qinghua GUO, Guangsuo YU. Spectral radiation characterization of OH*, NH₂* and NH* in ammonia/methane diffusion flame[J]. CIESC Journal, 2023, 74(11): 4710-4719.

段正巧, 龚岩, 郭庆华, 于广锁. 氨/甲烷扩散火焰中OH*、NH₂*和NH*光谱辐射特性研究[J]. 化工学报, 2023, 74(11): 4710-4719.

Figures/Tables 14

Fig.1 Flame chemiluminescence detection platform

Table 1 Experimental conditions

序号	CH₄/(L·min^-1)	NH₃/(L·min^-1)	$X N H 3$	O₂/(L·min^-1)	φ
1	0.30	0	0	0.60	1.0
2	0.27	0.03	0.1	0.34~0.84	0.6~1.5
3	0.24	0.06	0.2	0.32~0.79	0.6~1.5
4	0.21	0.09	0.3	0.29~0.73	0.6~1.5
5	0.18	0.12	0.4	0.27~0.68	0.6~1.5
6	0.15	0.15	0.5	0.25~0.62	0.6~1.5

Table 1 Experimental conditions

序号	CH₄/(L·min^-1)	NH₃/(L·min^-1)	$X N H 3$	O₂/(L·min^-1)	φ
1	0.30	0	0	0.60	1.0
2	0.27	0.03	0.1	0.34~0.84	0.6~1.5
3	0.24	0.06	0.2	0.32~0.79	0.6~1.5
4	0.21	0.09	0.3	0.29~0.73	0.6~1.5
5	0.18	0.12	0.4	0.27~0.68	0.6~1.5
6	0.15	0.15	0.5	0.25~0.62	0.6~1.5

Fig.2 Ammonia/methane diffusion flame photometry graph

Table 2 NH2*， NH* radical reactions

序号	NH₂*	序号	NH*
R1	NH₂* $̿$ NH₂+hv	R11	NH* $̿$ NH+hv
R2	NH₂*+M $̿$ NH₂+M	R12	NH*+NH₃ $̿$ NH+NH₃
R3	NH+H+M $̿$ NH₂*+M N₂/1.0/NH₃/2.5/AR/0.38/HE/0.36/CH₄/0.76/CO/1.16/H₂/1.14/	R13	NH*+M $̿$ NH+M O₂/1.0/NH₃/0.0/H₂O/5.3/C₂H₆/4.2/CH₄/2.3/CO/2.2/H₂/1.5/N₂/0.02/
R4	NH₂*+H₂ $̿$ NH₃+H	R14	NH*+H₂O $̿$ NH₂+OH
R5	NH+H₂ $̿$ NH₂+H	R15	NH*+H₂ $̿$ NH₂+H
R6	NH₂*+H₂O $̿$ NH₃+OH	R16	NH*+NH₃ $̿$ 2NH₂
R7	N₂+NH₂*+H $̿$ N₂(A)+NH₃	R17	NH*+H $̿$ N+H₂
R8	NH₂+N₂(A) $̿$ NH₂*+N₂	R18	N₂(A)+NH $̿$ N₂+NH*
R9	N₂H₄+H $̿$ NH₃+NH₂*	R19	CH+NO $̿$ NH*+CO
R10	N₂H₄+H $̿$ N₂H₃+H₂

Table 2 NH2*， NH* radical reactions

序号	NH₂*	序号	NH*
R1	NH₂* $̿$ NH₂+hv	R11	NH* $̿$ NH+hv
R2	NH₂*+M $̿$ NH₂+M	R12	NH*+NH₃ $̿$ NH+NH₃
R3	NH+H+M $̿$ NH₂*+M N₂/1.0/NH₃/2.5/AR/0.38/HE/0.36/CH₄/0.76/CO/1.16/H₂/1.14/	R13	NH*+M $̿$ NH+M O₂/1.0/NH₃/0.0/H₂O/5.3/C₂H₆/4.2/CH₄/2.3/CO/2.2/H₂/1.5/N₂/0.02/
R4	NH₂*+H₂ $̿$ NH₃+H	R14	NH*+H₂O $̿$ NH₂+OH
R5	NH+H₂ $̿$ NH₂+H	R15	NH*+H₂ $̿$ NH₂+H
R6	NH₂*+H₂O $̿$ NH₃+OH	R16	NH*+NH₃ $̿$ 2NH₂
R7	N₂+NH₂*+H $̿$ N₂(A)+NH₃	R17	NH*+H $̿$ N+H₂
R8	NH₂+N₂(A) $̿$ NH₂*+N₂	R18	N₂(A)+NH $̿$ N₂+NH*
R9	N₂H₄+H $̿$ NH₃+NH₂*	R19	CH+NO $̿$ NH*+CO
R10	N₂H₄+H $̿$ N₂H₃+H₂

Fig.3 NH2*, NH* radiation intensity and simulated mole fraction integration values

Fig.4 Ammonia/methane diffusion flame image

Fig.5 OH* relative radiation intensity distribution of ammonia/methane flames with different mixing ratios

Fig.6 NH2* relative radiation intensity distribution of ammonia/methane flames with different mixing ratios

Fig.7 NH* relative radiation intensity distribution of ammonia/methane flames with different mixing ratios

Fig.8 Relative peak intensity of OH*, NH2* and NH* at different equivalent ratios

Fig.9 Relative position of OH*, NH2* and NH*(XNH3= 0.1, φ = 1.0)

Fig.10 OH*, NH2* and NH* peak radiation intensity positions with various ammonia mixing ratio

Fig.11 NH2*, NH* reaction production rate at ammonia mixing ratio of 0.1

Fig.12 NH* reaction production rate integral

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Spectral radiation characterization of OH, NH₂ and NH* in ammonia/methane diffusion flame

氨/甲烷扩散火焰中OH、NH₂和NH*光谱辐射特性研究

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