不同燃料类型锅炉羰基化合物的排放特征

姚倩; 沈丽冉; 张春林; 白莉; 黄江荣; 刘军; 杨军; 王好; 王伯光

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中国环境科学 ›› 2020, Vol. 40 ›› Issue (2) : 573-581.

大气污染与控制

不同燃料类型锅炉羰基化合物的排放特征

姚倩¹, 沈丽冉^1,2, 张春林¹, 白莉², 黄江荣², 刘军², 杨军¹, 王好¹, 王伯光¹

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Characteristics of carbonyl compounds from boilers fired different types of fuel

YAO Qian¹, SHEN Li-ran^1,2, ZHANG Chun-lin¹, BAI Li², HUANG Jiang-rong², LIU Jun², YANG Jun¹, WANG Hao¹, WANG Bo-guang¹

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摘要

为探究不同燃料类型锅炉羰基化合物排放特征，选取以煤、生物质、石油焦和天然气为燃料的14台工业锅炉和2台燃煤电站锅炉作为研究对象，采用气袋-PFPH衍生-GC/MS方法采集和分析烟气中的21种羰基化合物.结果表明，不同燃料类型锅炉烟气中羰基化合物呈现明显差异（One-way ANOVA，F=4.458，P=0.028<0.05），其中羰基化合物质量浓度（9%基准氧量）排序是石油焦 > 电站锅炉 > 煤 > 天然气 > 生物质，分别为（6306.25±1335.35），（5745.96±2864.62），（4784.85±1698.20），（3589.51±1534.676），（1341.18±616.46）μg/m³.不同燃料类型的锅炉烟气中羰基化合物组分特征有明显差异性，但甲醛、乙醛、丙酮和丙醛等低分子量的羰基化合物均占比较大，燃石油焦、燃煤电站、燃煤、燃天然气和燃生物质锅炉中低碳羰基化合物总占比分别达到87.56%，91.36%，92.94%，78.70%和45.84%.最后，采用最大增量反应活性（MIR）和OH消耗速率评价烟气中羰基化合物物种的化学反应活性，结果表明，甲醛、丙醛、乙醛等低碳羰基化合物为关键活性物种.

Abstract

To explore the emission characteristics of carbonyl compounds (CCs) from boilers with different fuel types, the exhausts from the stacks of 14industrial boilers, whose fuel type included coal, biomass, petroleum coke and natural gas, and 2coal-fired utility boilers were sampled in the study. 21CCs were analyzed by a PFPH-derivatization-GC/MS method. The results showed that the composition of CCs in the exhausts varied significantly among different fuel types of boilers (One-way ANOVA, F=4.458, P=0.028<0.05). The total mass concentration of CCs (based on 9% oxygen content) was ranked as petroleum-coke-fired boilers > coal-fired utility boilers > coal-fired industrial boilers > gas-fired boilers > biomass-fired boilers, with the total mass concentrations of (6306.25±1335.35), (5745.96±2864.62),(5313.57±2959.36), (2461.38±1052.35), and (1341.18±616.46) μg/m³, respectively. Furthermore, among all types of boilers, low-molecular-mass-weight CCs, (e.g. formaldehyde, aldehyde, acetone and propanal) were the most important contributors to the total CCs of the exhaust, which occupied 87.56%, 91.36%, 92.94%, 78.70%, and 45.84% in the exhausts of petroleum-coke-fired, coal-fired utility, coal-fired industrial, gas-fired boilers and biomass-fired boilers, respectively. At last, ozone formation potential (OFP) was evaluated by maximum incremental reactivity (MIR) and total hydroxyl radical (OH) reactivity by CCs, respectively, revealing that formaldehyde, propionaldehyde, acetaldehyde are the key species with high OFP and (OH) reactivity.

导出引用

姚倩, 沈丽冉, 张春林, 白莉, 黄江荣, 刘军, 杨军, 王好, 王伯光. 不同燃料类型锅炉羰基化合物的排放特征[J]. 中国环境科学. 2020, 40(2): 573-581

YAO Qian, SHEN Li-ran, ZHANG Chun-lin, BAI Li, HUANG Jiang-rong, LIU Jun, YANG Jun, WANG Hao, WANG Bo-guang. Characteristics of carbonyl compounds from boilers fired different types of fuel[J]. China Environmental Science. 2020, 40(2): 573-581

中图分类号： X701.3

参考文献

[1] Yang Z, Cheng H R, Wang Z W, et al. Chemical characteristics of atmospheric carbonyl compounds and source identification of formaldehyde in Wuhan, Central China[J]. Atmospheric Research, 2019,228(2019):95-106.
[2] Bunkoed O, Thavarungkul P, Thammakhet C, et al. A simple and high collection efficiency sampling method for monitoring of carbonyl compounds in a workplace environment[J]. Journal of Environmental Science & Health Part A Toxic/hazardous Substances & Environmental Engineering, 2012,47(2):167-175.
[3] Kumar A, Alaimo C P, Horowitz R, et al. Volatile organic compound emissions from green waste composting:Characterization and ozone formation[J]. Atmospheric Environment, 2011,45(10):1841-1848.
[4] WHO. Air quality guidelines for Europe. Regional office for Europe, Copenhagen, Denmark[Z]. 2000.
[5] Liu Z, Wang Y H, Vrekoussis M, et al. Exploring the missing source of glyoxal (CHOCHO) over China[J]. Geophysical Research Letters, 2012,39(2012):L10812.
[6] Fu T M, Jacob D J, Wittrock F, et al. Global budgets of atmospheric glyoxal and methylglyoxal, and implications for formation of secondary organic aerosols[J]. Journal of Geophysical Research-Atmospheres, 2008,113(D15):1596-1598.
[7] Li J, Zhang M, Tang G, et al. Investigating missing sources of glyoxal over China using a regional air quality model (RAMS-CMAQ)[J]. Journal of Environmental Sciences, 2018,71(9):S100107421732212X.
[8] Yuan B, Liu Y, Shao M, et al. Biomass Burning Contributions to Ambient VOCs Species at a Receptor Site in the Pearl River Delta (PRD), China[J]. Environmental Science & Technology, 2010,44(12):4577-4582.
[9] Andreae M O, Merlet P. Emission of trace gases and aerosols from biomass burning[J]. Globl Biogeochem Cycle, 2001,15(4):955-966.
[10] Wang H L, Lou S R, Huang C, et al. Source Profiles of Volatile Organic Compounds from Biomass Burning in Yangtze River Delta, China[J]. Aerosol Air Quality Research, 2014,14(3):818-828.
[11] Mcdonald J D, Zielinska B, Fujita E M, et al. Fine particle and gaseous emission rates from residential wood combustion[J]. Environmental Science & Technology, 2000,34(11):2080-2091.
[12] Ban-Weiss G A, Mclaughlin J P, Harley R A, et al. Carbonyl and nitrogen dioxide emissions from gasoline- and diesel-powered motor vehicles[J]. Environmental Science & Technology, 2008,42(11):3944-3950.
[13] Lu Y Y, Yi L, Han Z, et al. Evaluation of Volatile Organic Compounds and Carbonyl Compounds Present in the Cabins of Newly Produced, Medium- and Large-Size Coaches in China[J]. International Journal of Environmental Research & Public Health, 2016,13(2016):596.
[14] Pang X B, Lewis A C. Carbonyl compounds in gas and particle phases of mainstream cigarette smoke[J]. Environmental Science & Technology, 2011,409(23):5000-5009.
[15] 秦存永,何爱民,赵晖,等.高效液相色谱法测定卷烟燃烧生成的羰基化合物的分布[J]. 食品工业, 2017,38(1):289-292. Cun-Yong Q, Ai-Min H, Hui Z, et al. The Determination of Distribution on Major Carbonyl Compounds during Cigarette Burning by HPLC[J]. Food Industry, 2017,38(1):289-292.
[16] 马慧莲,金静,李云,等.热脱附-气相色谱-质谱法应用于工业源废气中挥发性有机物的目标和非目标筛查[J]. 色谱, 2017,35(10):1094-1099. Ma H, Jin J, Li Y, et al. Target and non-target screening of volatile organic compounds in industrial exhaust gas using thermal desorption-gas chromatography-mass spectrometry[J]. Chinese Journal of Chromatography, 2017,35(10):1094-1099.
[17] 张立志,高健,赵黛青,等.含氧燃料燃烧中燃料氧迁移路径及含氧中间体生成特性[J]. 物理化学学报, 2011,27(8):1809-1815. Zhang L Z, Gao J, Zhao D Q, et al. Migration Pathways of Oxygen and the Formation of Oxygenated Intermediates in Oxygenated Fuel Combustion[J]. Acta Physico-Chimica Sinica, 2011, 27(8):1809-1815.
[18] Gysel N, Welch W A, Chen C L, et al. Particulate matter emissions and gaseous air toxic pollutants from commercial meat cooking operations[J]. Journal of Environmental Sciences, 2018,65(2018):162-170.
[19] Chen J M, Li C L, Ristovski Z, et al. A review of biomass burning:Emissions and impacts on air quality, health and climate in China[J]. Science of the Total Environment, 2017,579(2017):1000-1034.
[20] 刘亚男,钟连红,闫静,等.民用燃料燃烧碳质组分及VOCs排放特征[J]. 中国环境科学, 2019,39(4):1412-1418. Liu Y, Zhong L, Yan J, et al. Carbon compositions and VOCs emission characteristics of civil combustion fuels[J]. China Environmental Science, 2019,39(4):1412-1418.
[21] 郭文凯,刘镇,刘文博,等.兰州生物质燃烧VOCs排放特征及其大气环境影响[J]. 中国环境科学, 2019,39(1):40-49. Guo W, Liu Z, Liu W, et al. The characteristics of VOCs emission from biomass burning and its influence on atmospheric environment in Lanzhou City[J]. China Environmental Science, 2019,39(1):40-49.
[22] Zarzana K J, Min K E, Washenfelder R A, et al. Emissions of Glyoxal and Other Carbonyl Compounds from Agricultural Biomass Burning Plumes Sampled by[J]. Environmental Science & Technology, 2017,51(20):11761-11770.
[23] Shi J W, Deng H, Bai Z P, et al. Emission and profile characteristic of volatile organic compounds emitted from coke production, iron smelt, heating station and power plant in Liaoning Province, China[J]. Science of the Total Environment, 2015,515(2015):101-108.
[24] 沈丽冉,张春林,吴昌达,等.生物质锅炉羰基化合物排放特征分析[J]. 2018,38(2):490-498. Shen L, Zhang C, Wu C, et al. Emission characteristics of carbonyl compounds emitted from biomass-fired-boilers[J]. China Environmental Science, 2018,38(2):490-498.
[25] HJ/T397-2007固定源废气监测技术规范[S]. HJ/T397-2007 Technical specifications for emission monitoring of stationary source[S].
[26] Ho S S H, Yu J Z. Determination of airborne carbonyls:Comparison of a thermal desorption/GC method with the standard DNPH/HPLC method[J]. Environmental Science & Technology, 2004,38(3):862-870.
[27] Li J, Feng Y L, Xie C J, et al. Determination of gaseous carbonyl compounds by their pentafluorophenyl hydrazones with gas chromatography/mass spectrometry[J]. Analytica Chimica Acta, 2009, 635(1):84-93.
[28] Pang X B, Lewis A C, Hamilton J F. Determination of airborne carbonyls via pentafluorophenylhydrazine derivatisation by GC-MS and its comparison with HPLC method[J]. Environmental Science & Technology, 2011,85(1):406-414.
[29] 周咪,王伯光,赵德骏,等.城市污水处理厂恶臭挥发性羰基化合物的排放特征[J]. 环境科学, 2011,32(12):3571-3576. Zhou M, Wang B G, Zhao D J, et al. Source emission characteristics of malodorous volatile organic carbonyls from a municipal sewage treatment plant[J]. Environmental Science, 2011,32(12):3571-3576.
[30] GB13271-2014锅炉大气污染物排放标准[S]. GB13271-2014 Emission standard of air pollutants for boiler[S].
[31] GB13223-2011火电厂大气污染物排放标准[S]. GB13223-2011 Emission standard of air pollutants for thermal power plants[S].
[32] 魏巍.中国人为源挥发性有机化合物的排放现状及未来趋势[D]. 北京:清华大学, 2009 Wei W. Study on current and future anthropogenic emissions of volatile organic compounds in China[D]. Beijing:Tsinghua University, 2009.
[33] Mo Z W, Shao M, Lu S H. Compilation of a source profile database for hydrocarbon and OVOC emissions in China[J]. Atmospheric Environment, 2016,143(2016):209-217.
[34] 李兴华,王书肖,郝吉明.民用生物质燃烧挥发性有机化合物排放特征[J]. 环境科学, 2011,32(12):3515-3521. Li X H, Wang S X, Hao J M. Characteristics of volatile organic compounds (VOCs) emitted from biofuel combustion in China[J]. Environmental Science, 2011,32(12):3515-3521.
[35] Feng Y L, Xiong B, Cui M U, et al. Emissions of volatile organic compounds and carbonyl compounds from residential coal combustion in China[J]. Advances in Manufacturing, 2010,14(2):79-82.
[36] 姬亚芹.城市空气颗粒物源解析土壤风沙尘成分谱研究[D]. 天津:南开大学, 2006 JI Yaqin. Study on the soil dust profiles for source apportionment of ambient particulate matter[D]. Tianjin:Nankai University, 2006.
[37] Cheng S Y, Wang G, Lang J L, et al. Characterization of volatile organic compounds from different cooking emissions[J]. Atmospheric Environment, 2016,145(2016):299-307.
[38] Carter W P L. Development of the SAPRC-07chemical mechanism[J]. Atmospheric Environment, 2010,44(40):5324-5335.
[39] Atkinson R, Arey J. Atmospheric degradation of volatile organic compounds[J]. Chemical Reviews, 2003,103(12):4605-4638.