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温度是燃烧过程中影响反应路径和速率的重要参数, 决定着燃烧和能量交换效率, OH, NH, NO等组分参与燃烧中的关键基元反应, 并影响NOx污染物的生成. 因此, 温度和OH, NH, NO浓度的同步测量对于判断燃烧状态、研究反应机理和排放特性具有重要意义. 本文搭建了高空间分辨率的宽带紫外吸收光谱测量系统, 实现了火焰温度和OH, NH, NO浓度的同步测量, 并对3种组分宽带吸收光谱的温度灵敏度和浓度检出限进行了定量分析. 随后, 利用所建立的测量方法对NH3/CH4/air常压平面预混火焰的温度和OH, NH, NO浓度的高度分布进行了高精度测量: NH的1σ检出限达到1.8×10–9 m (1560 K), 在常压火焰实现了10–9量级的NH吸收光谱测量; OH和NO的1σ检出限分别达到60×10–9 m (1590 K) 和1×10–6 m (1380 K), 也明显优于现有的红外激光吸收光谱测量结果. 实验所得温度和OH, NO, NH浓度分布曲线与基于Okafor等机理的计算流体动力学预测结果非常符合, 验证了基于宽带紫外吸收光谱方法的温度和组分浓度同步测量效果.Temperature is an important parameter influencing the combustion reaction path and rate and determining the combustion and energy exchange efficiency. The OH, NH, NO and other species are involved in the key elementary reactions of combustion and determine the generation of NOx pollutants. Therefore, temperature and concentration measurements of OH, NH, and NO are of great significance for combustion diagnostics and research on reaction or emission mechanisms. In this work, a measurement system with high spatial resolution based on broadband ultraviolet absorption spectroscopy is established to realize simultaneous measurements of the temperature and concentrations of OH, NH, and NO in flames. Low detection limits of these three species are achieved by using the established measurement method. The 1σ detection limit of NH is 1.8 ppb·m (1560 K), which is realized for the first time in atmospheric-pressure flames using absorption spectroscopy. The 1σ detection limits of OH and NO are 60 ppb·m (1590 K) and 1 ppm·m (1380 K), respectively, which are obviously better than the existing results obtained by using infrared laser absorption spectroscopy. Then, the distributions of temperatures and concentrations of OH, NO and NH are acquired at various heights in an atmospheric-pressure NH3/CH4/air premixed flat flame with a high spatial resolution of nearly 0.1 mm. The broadband absorption spectra of OH and NH are acquired simultaneously inside the flame front, and the spectra of OH and NO are acquired simultaneously above the flame front. Inside or near the flame front, the temperatures deduced from the spectra of OH, NH, and NO are consistent, verifying the ability of these three species to be used to measure temperature. In addition, OH, NH, and NO are found to be suitable for different regions in combustion. The OH absorption is suitable for the post-combustion region with temperatures higher than 1000 K, the NH absorption can be used to acquire the temperature inside the flame front in complex combustion, and the NO absorption was able to provide the temperature in the region before or outside combustion at lower temperatures. Additionally, the experimental temperature and concentration profiles are in good agreement with the computational fluid dynamics predictions based on the mechanism, exhibiting the accuracy of the simultaneous temperature and concentration measurements by using broadband ultraviolet absorption spectra. Moreover, the differences in temperature and OH concentration between experiments and simulations indicate that the carbon sub-mechanism in the mechanism given by Okafor et al. [Okafor E C, Naito Y, Colson S, Ichikawa A, Kudo T, Hayakawa A, Kobayashi H
2018 Combust. Flame 187 185 ] should be further improved for more accurate predictions of NH3/CH4 combustion.-
Keywords:
- broadband ultraviolet absorption spectroscopy /
- combustion diagnostics /
- temperature measurements /
- concentration measurements
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图 1 1800 K条件下待测组分OH, NO, NH及三种主要燃烧产物CO, CO2, H2O线强度. 其中OH, NO, NH数据来自EXOMOL数据库; CO, CO2, H2O数据来自HITEMP数据库
Fig. 1. Line-strengths of OH, NO, NH and CO, CO2, H2O at 1800 K. The data of OH, NO, NH are taken from the EXOMOL database, and that of CO, CO2, and H2O are taken from the HITEMP database.
图 2 不同温度下仿真的峰值归一化的吸收率和1700 K下线强度大于最大线强1%的谱线的下能态能级 (a) OH; (b) NH; (c) NO
Fig. 2. Simulated peak normalized absorbance at various temperatures and lower-state energies of lines with line-strength more than 1% of the maximum line-strength at 1700 K: (a) OH; (b) NH; (c) NO.
图 3 仿真信噪比为100时不同温度条件下温度拟合的相对标准差
Fig. 3. The relative standard deviation of fitted temperature with the simulated signal-to-noise ratio of 100 at various temperatures.
图 4 宽带吸收的光路布置和McKenna燃烧器供水供气系统示意图
Fig. 4. Schematic of the optical arrangement and the system of the McKenna burner with gas supply and cooling-water.
图 5 CFD网格和边界条件设置示意图、OH云图和火焰照片
Fig. 5. CFD setup of the grid and boundary conditions, together with the contour of OH mole fraction and the photo of the flame.
图 6 NH峰值所在高度(HAB = 1.07 mm)的(a) OH和 (b) NH的测量与拟合光谱, 光谱分辨率均为30 pm
Fig. 6. Measured and fitted spectra of (a) OH and (b) NH at the same height of the NH peak value (HAB = 1.07 mm) with the instrumental resolution of 30 pm.
图 7 火焰面内不同高度下两组实验中OH和NH拟合及CFD模拟的温度和摩尔分数分布
Fig. 7. The temperatures and concentrations of OH and NH in two experimental groups and simulation results from CFD at various heights inside the flame front.
图 8 近火焰面的高度(HAB = 1.38 mm)下(a) OH和 (b) NO以及远离火焰面的高度(HAB = 12.63 mm)下 (c) OH和(d) NO的测量和拟合光谱, 310 nm附近OH光谱分辨率30 pm, 225 nm附近NO光谱分辨率34 pm
Fig. 8. Measured and fitted spectra near the flame (HAB = 1.38 mm) of (a) OH and (b) NO and the spectra far away the flame (HAB = 12.63 mm) of (c) OH and (d) NO with the instrumental resolution of 30 pm at 310 nm and of 34 pm at 225 nm.
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[1] Anderson T N, Lucht R P, Priyadarsan S, Annamalai K, Caton J A 2007 Appl. Opt. 46 3946
Google Scholar
[2] Wang S K, Hanson R K 2018 Appl. Phys. B 124 37
Google Scholar
[3] Somarathne K, Okafor E C, Sugawara D, Hayakawa A, Kobayashi H 2021 Proc. Combust. Inst. 38 5163
Google Scholar
[4] Zhang M, An Z H, Wang L, Wei X T, Jianayihan B, Wang J H, Huang Z H, Tan H Z 2021 Int. J. Hydrogen Energy 46 21013
Google Scholar
[5] Lamoureux N, Gasnot L, Desgroux P 2019 Proc. Combust. Inst. 37 1313
Google Scholar
[6] Li S, Zhang S S, Zhou H, Ren Z Y 2019 Fuel 237 50
Google Scholar
[7] Bürkle S, Dreizler A, Ebert V, Wagner S 2018 Fuel 212 302
Google Scholar
[8] Peng Z M, Du Y J, Ding Y J 2020 Sensors 20 616
Google Scholar
[9] Cheong K P, Ma L H, Wang Z, Ren W 2019 Appl. Spectrosc. 73 529
Google Scholar
[10] Hanson R K, Davidson D F 2014 Prog. Energy Combust. Sci. 44 103
Google Scholar
[11] He D, Ding Y J, Shi L, Zheng D, Peng Z M 2021 Combust. Flame 232 111537
Google Scholar
[12] Shang Y L, Wang Z, Ma L H, Shi J C, Ning H B, Ren W, Luo S N 2021 Proc. Combust. Inst. 38 1745
Google Scholar
[13] Ma L, Li X S, Sanders S T, Caswell A W, Roy S, Plemmons D H, Gord J R 2013 Opt. Express 21 1152
Google Scholar
[14] Azimov U, Kawahara N, Tomita E 2016 Fuel 182 807
Google Scholar
[15] Cassady S J, Peng W Y, Strand C L, Dausen D F, Codoni J R, Brophy C M, Hanson R K 2021 Proc. Combust. Inst. 38 1719
Google Scholar
[16] Goldenstein C S, Spearrin R M, Jeffries J B, Hanson R K 2017 Prog. Energy Combust. Sci. 60 132
Google Scholar
[17] Gao Z W, Gao G Z, Cai T D 2021 Appl. Phys. B 127 158
Google Scholar
[18] Anderson W R, Decker L J, Kotlar A J 1982 Combust. Flame 48 179
Google Scholar
[19] Branch M C, Sadeqi M E, Alfarayedhi A A, Vantiggelen P J 1991 Combust. Flame 83 228
Google Scholar
[20] Derzy I, Lozovsky V A, Ditzian N, Rahinov I, Cheskis S 2000 Proc. Combust. Inst. 28 1741
Google Scholar
[21] Bruggeman P, Cunge G, Sadeghi N 2012 Plasma Sources Sci. Technol. 21 035019
Google Scholar
[22] Du Y J, Nayak G, Oinuma G, Ding Y J, Peng Z M, Bruggeman P J 2017 Plasma Sources Sci. Technol. 26 095007
Google Scholar
[23] Schroter S, Wijaikhum A, Gibson A R, West A, Davies H L, Minesi N, Dedrick J, Wagenaars E, de Oliveira N, Nahon L, Kushner M J, Booth J P, Niemi K, Gans T, O'Connell D 2018 Phys. Chem. Chem. Phys. 20 24263
Google Scholar
[24] Brisset A, Gibson A R, Schroter S, Niemi K, Booth J P, Gans T, O'Connell D, Wagenaars E 2021 J. Phys. D:Appl. Phys. 54 285201
Google Scholar
[25] Sepman A, Gullberg M, Wiinikka H 2020 Appl. Phys. B 126 100
Google Scholar
[26] Lempert W R 1988 Combust. Flame 73 89
Google Scholar
[27] 刘宇, 刘文清, 阚瑞峰, 司福祺, 许振宇, 胡仁志, 谢品华 2011 光谱学与光谱分析 31 2659
Google Scholar
Liu Y, Liu W Q, Kan R F, Si F Q, Xu Z Y, Hu R Z, Xie P H 2011 Spectrosc. Spectr. Anal. 31 2659
Google Scholar
[28] Weng W B, Alden M, Li Z S 2019 Anal. Chem. 91 10849
Google Scholar
[29] Vilches T B, Weng W B, Glarborg P, Li Z S, Thunman H, Seemann M 2020 Fuel 273 117762
Google Scholar
[30] Weng W B, Li S, Alden M, Li Z S 2021 Appl. Spectrosc. 75 1168
Google Scholar
[31] White L, Gamba M 2018 J. Quant. Spectrosc. Radiat. Transfer 209 73
Google Scholar
[32] Yang X Y, Peng Z M, Ding Y J, Du Y J 2021 Fuel 288 119666
Google Scholar
[33] Okafor E C, Naito Y, Colson S, Ichikawa A, Kudo T, Hayakawa A, Kobayashi H 2018 Combust. Flame 187 185
Google Scholar
[34] Gordon I E, Rothman L S, Hargreaves R J, et al. 2022 J. Quant. Spectrosc. Radiat. Transfer 277 107949
Google Scholar
[35] Rothman L S, Gordon I E, Barber R J, Dothe H, Gamache R R, Goldman A, Perevalov V I, Tashkun S A, Tennyson J 2010 J. Quant. Spectrosc. Radiat. Transfer 111 2139
Google Scholar
[36] Tennyson J, Yurchenko S N, Al-Refaie A F, et al. 2020 J. Quant. Spectrosc. Radiat. Transfer 255 107228
Google Scholar
[37] Girard J J, Choudhary R, Hanson R K 2018 J. Quant. Spectrosc. Radiat. Transfer 221 194
Google Scholar
[38] Rocha R C, Zhong S H, Xu L L, Bai X S, Costa M, Cai X, Kim H, Brackmann C, Li Z S, Alden M 2021 Energy Fuels 35 7179
Google Scholar
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