薪柴燃烧溶解性棕色碳排放特征及光学性质

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摘要对农村薪柴（杨木和毛竹）燃烧排放的4类溶解性棕色碳（BrC）组分，包括水溶性有机物（WSOM）、水溶性类腐殖质（HULIS_WS）、碱溶性有机物（ASOM）和碱溶性类腐殖质（HULIS_AS）的组成特征和光学性质进行了初步研究.结果显示，薪柴燃烧排放出大量的BrC，其中BrC_T（WSOM+ASOM）占烟气PM_2.5质量的46%~56%，排放因子为（7.5~16）g/kg.HULIS是薪柴燃烧排放BrC的重要组分，占BrC_T的44%~46%.4类BrC的特征吸收指数（SUVA₂₅₄）、光吸收效率（MAE₃₆₅）和Ångström指数（AAE）值分别为1.9~4.0m²/g、0.4~2.1m²/g和6.2~11.1，说明薪柴燃烧排放BrC具有较高的芳香度、较强的光吸收能力且其光吸收具有较强的波长依赖性.三维荧光光谱分析结果显示，薪柴燃烧排放BrC主要以类蛋白荧光物质组成为主，这与雨水和大气气溶胶中水溶性BrC以类腐殖质荧光物质组成为主的特征存在显著差异.相关性分析结果显示，BrC的MAE₃₆₅与HIX和SUVA₂₅₄呈现显著的正相关性，与E₂/E₃、FI、BIX和β：α呈现显著的负相关性，说明薪柴燃烧排放BrC的光吸收特性与其芳香性、腐殖化程度、自生源贡献和新鲜度等紧密相关.本研究结果有助于进一步认识生物质燃烧BrC的排放特征，为探索大气BrC的来源和环境效应提供数据基础和科学依据.

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关键词 ：薪柴燃烧, 棕色碳, 排放特征, 光吸收特性, 荧光光谱特性

Abstract：The study was aimed to investigate the emission characteristics and optical properties of primary brown carbon (BrC), including water-soluble organic matters (WSOM), water-soluble humic like substances (HULIS_WS), alkaline-soluble organic matters (ASOM), alkaline-soluble HULIS (HULIS_AS), emitted from household residential wood combustion. The results showed that residential wood combustion emitted large amounts of BrC. Among them, BrC_T (WSOM + ASOM) were observed to make up 46%~56% of total smoke PM_2.5 mass, and the emission factors of them were 7.5~16g/kg. HULIS were important light absorber in primary BrC, which accounted for 44%~46% of BrC_T. The SUVA₂₅₄, MAE₃₆₅ and AAE values for primary BrC were 1.9~4.0m²/g, 0.4~2.1m²/gand 6.2~11.1, respectively, indicating that the primary BrC emitted from wood combustion exhibited high aromaticity, strong light absorbing capacity and its light absorption presented strong wavelength dependence. 3DEEM results showed that the protein-like substances were dominant fluorophores for primary BrC fractions. It was significantly different from the fluorescent characteristics for WSOM in rainwater and atmospheric aerosols, in which the humic-like substances were predominant fluorophores. The correlation analysis revealed that MAE₃₆₅ present strong positive correlations with HIX and SUVA₂₅₄, while strong negative correlations were found with E₂/E₃, FI, BIX and β:α. It implied that the light absorption of primary BrC emitted from residential wood combustion were greatly related to their aromaticity, humification degree, autochthonous and freshness characteristics. The results obtained in this study are helpful to better understand the emission characteristics of BrC from BB, and also can provide such deep insight into the sources and environment effects of atmospheric BrC.

Key words： residential wood combustion brown carbon emission characteristics light absorption fluorescence spectral properties

收稿日期: 2019-01-28

PACS:

X513

基金资助:国家自然科学基金资助项目（41705107，41673117）；安徽省科技重大专项（16030701102）；安徽省教育厅重点项目（KJ2017A520）；安徽省自然科学基金资助项目（1808085MB49，1708085QD85）

通讯作者: 宋建中,副研究员,songjzh@gig.ac.cn E-mail: songjzh@gig.ac.cn

作者简介: 范行军(1987-),男,安徽六安人,讲师,博士,主要研究方向为大气气溶胶中棕色碳的光学特征和来源解析.发表论文10篇.

引用本文:

范行军, 操涛, 余旭芳, 宋建中, 王艳, 肖新, 谢越, 李飞跃. 薪柴燃烧溶解性棕色碳排放特征及光学性质[J]. 中国环境科学, 2019, 39(8): 3215-3224. FAN Xing-jun, CAO Tao, YU Xu-fang, SONG Jian-zhong, WANG Yan, XIAO Xin, XIE Yue, LI Fei-yue. Emission characteristics and optical properties of extractable brown carbon from residential wood combustion. CHINA ENVIRONMENTAL SCIENCECE, 2019, 39(8): 3215-3224.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2019/V39/I8/3215

[1]	闫才青,郑玫,张远航.大气棕色碳的研究进展与方向[J]. 环境科学, 2014,35(11):4404-4414. Yan C Q, Zheng M, Zhang Y H. Research progress and direction of atmospheric brown carbon[J]. Environmental science, 2014,35(11):4404-4414.
[2]	支国瑞,蔡竟,杨俊超,等.棕色碳气溶胶来源、性质、测量与排放估算[J]. 环境科学研究, 2015,28(12):1797-1814. Zhi G R, Cai J, Yang J C, et al. Origin, properties, measurement and emission estimation of brown carbon aerosols[J]. Research of Environmental Sciences, 2015,28(12):1797-1814.
[3]	Andreae M O, Gelencser A. Black carbon or brown carbon? The nature of light-absorbing carbonaceous aerosols[J]. Atmospheric Chemistry and Physics, 2006,6:3131-3148.
[4]	Liu J, Bergin M, Guo H, et al. Size-resolved measurements of brown carbon in water and methanol extracts and estimates of their contribution to ambient fine-particle light absorption[J]. Atmospheric Chemistry and Physics, 2013,13(24):12389-12404.
[5]	Yan C, Zheng M, Sullivan A P, et al. Chemical characteristics and light-absorbing property of water-soluble organic carbon in Beijing:Biomass burning contributions[J]. Atmospheric Environment, 2015, 121:4-12.
[6]	Hecobian A, Zhang X, Zheng M, et al. Water-Soluble Organic Aerosol material and the light-absorption characteristics of aqueous extracts measured over the Southeastern United States[J]. Atmospheric Chemistry and Physics, 2010,10(13):5965-5977.
[7]	Du Z, He K, Cheng Y, et al. A yearlong study of water-soluble organic carbon in Beijing Ⅱ:Light absorption properties[J]. Atmospheric Environment, 2014,89:235-241.
[8]	段菁春,毕新慧,谭吉华,等.广州灰霾期大气颗粒物中多环芳烃粒径的分布[J]. 中国环境科学, 2006,26(1):6-10. Duan J C, Bi X H, Tan J H, et al. The particle diameter distribution of polycyclic aromatic hydrocarbons (PAHs) in atmospheric particle during haze period in Guangzhou[J]. China Environmental Science, 2006,26(1):6-10.
[9]	崔杰,黄晓锋,袁金凤,等.基于在线观测的大气PM2.5中棕色碳吸光贡献估算[J]. 中国环境科学, 2017,37(2):401-406. Cui J, Huang X F, Yuan J F, et al. Estimation of light absorption by brown carbon in PM2.5 based on on-line measurement[J]. China Environmental Science, 2017,37(2):401-406.
[10]	Feng Y, Ramanathan V, Kotamarthi V R. Brown carbon:a significant atmospheric absorber of solar radiation?[J] Atmospheric Chemistry and Physics, 2013,13(17):8607-8621.
[11]	Laskin A, Laskin J, Nizkorodov S A. Chemistry of Atmospheric Brown Carbon[J]. Chemical Reviews, 2015,115(10):4335-4382.
[12]	Chen Y, Bond T C. Light absorption by organic carbon from wood combustion[J]. Atmospheric Chemistry and Physics, 2010,10(4):1773-1787.
[13]	Fan X, Wei S, Zhu M, et al. Comprehensive characterization of humic-like substances in smoke PM2.5 emitted from the combustion of biomass materials and fossil fuels[J]. Atmospheric Chemistry and Physics, 2016,16(20):13321-13340.
[14]	Cheng Y, He K B, Zheng M, et al. Mass absorption efficiency of elemental carbon and water-soluble organic carbon in Beijing, China[J]. Atmospheric Chemistry and Physics, 2011,11(22):11497-11510.
[15]	Kirillova E N, Andersson A, Han J, et al. Sources and light absorption of water-soluble organic carbon aerosols in the outflow from northern China[J]. Atmospheric Chemistry and Physics, 2014,14(3):1413-1422.
[16]	梁俭,江韬,魏世强,等.夏、冬季降雨中溶解性有机质(DOM)光谱特征及来源辨析[J]. 环境科学, 2015,36(3):888-897. Liang J, Jiang T, Wei S Q, et al. Absorption and fluorescence characteristics of dissolved organic matter (DOM) in rainwater and sources analysis in summer and winter season[J]. Environmental Science, 2015,36(3):888-897.
[17]	孙建中,支国瑞,陈颖军,等.居民生活用煤和生物质棕色碳排放因子研究[J]. 环境科学与技术, 2016,39(S1):338-345. Sun J Z, Zhi G R, Chen Y J, et al. Measurement of brown carbon emission factors for household use of coal and biomass in China[J]. Environmental Science & Technology, 2016,39(S1):338-345.
[18]	蔡竟,支国瑞,陈颖军,等.中国秸杆焚烧及民用燃煤棕色碳排放的初步研究[J]. 环境科学研究, 2014,27(5):455-461. Cai J, Zhi G R, Chen Y J,et al. A preliminary study on brown carbon emissions from open agricultural biomass burning and residential coal combustion in China[J]. Research of Environmental Sciences, 2014,27(5):455-461.
[19]	Fan X, Li M, Cao T, et al. Optical properties and oxidative potential of water-and alkaline-soluble brown carbon in smoke particles emitted from laboratory simulated biomass burning[J]. Atmospheric Environment, 2018,194:48-57.
[20]	Park S S, Yu J. Chemical and light absorption properties of humic-like substances from biomass burning emissions under controlled combustion experiments[J]. Atmospheric Environment, 2016,136:114-122.
[21]	韦思业,苏玉红,沈国锋,等.农村室内薪柴燃烧的颗粒物和炭黑排放因子[J]. 生态毒理学报, 2013,8(1):29-36. Wei S Y, Su Y H, Shen G F, et al. Emission factors of particulate matter and elemental carbon from rural residential wood combustion[J]. Asian Journal of Ecotoxicology, 2013,8(1):29-36.
[22]	Baduel C, Voisin D, Jaffrezo J L. Seasonal variations of concentrations and optical properties of water soluble HULIS collected in urban environments[J]. Atmospheric Chemistry and Physics, 2010,10(9):4085-4095.
[23]	Fan X, Song J, Peng P. Comparison of isolation and quantification methods to measure humic-like substances (HULIS) in atmospheric particles[J]. Atmospheric Environment, 2012,60:366-374.
[24]	Cheng Y, He K, Du Z, et al. The characteristics of brown carbon aerosol during winter in Beijing[J]. Atmospheric Environment, 2016,127:355-364.
[25]	范行军,余旭芳,操涛,等.广州冬季气溶胶中水溶性有机物和类腐殖质的吸光性和荧光光谱特性[J]. 环境科学, 2019,40(2):532-539. Fan X J, Yu X F, Cao T, et al. Light absorption and fluorescence characteristics of atmospheric water-soluble organic compounds and humic-like substances during the winter season in Guangzhou. Environmental Science, 2019,40(2):532-539.
[26]	周石磊,张艺冉,黄廷林,等.基于UV-vis及EEMs解析周村水库夏秋季降雨不同相对分子质量DOM的光谱特征及来源[J]. 环境科学, 2019,40(1):172-184. Zhou S L, Zhang Y R, Huang T L, et al. Spectral characteristics and sources of dissolved organic matter with different relative molecular weight from rainwater from summer and autumn in the zhoucun reservoir based on UV-Vis and EEMs. Environmental Science, 2019, 40(1):172-184.
[27]	Kothawala D N, von Wachenfeldt E, Koehler B, et al. Selective loss and preservation of lake water dissolved organic matter fluorescence during long-term dark incubations[J]. Science of the Total Environment, 2012,433:238-246.
[28]	祝斌,朱先磊,张元勋,等.农作物秸秆燃烧PM2.5排放因子的研究[J]. 环境科学研究, 2005,18(2):29-33. Zhu B, Zhu X L, Zhang Y X, et al. Emission factor of PM2.5 from crop straw burning[J]. Research of Environmental Sciences, 2005,18(2):29-33.
[29]	Hong L, Liu G, Zhou L, et al. Emission of organic carbon, elemental carbon and water-soluble ions from crop straw burning under flaming and smoldering conditions[J]. Particuology, 2017,31:181-190.
[30]	Peuravuori J, Pihlaja K. Isolation and characterization of natural organic matter from lake water:Comparison of isolation with solid adsorption and tangential membrane filtration[J]. Environment International, 1997,23(4):441-451.
[31]	Yuan J F, Huang X F, Cao L M, et al. Light absorption of brown carbon aerosol in the PRD region of China[J]. Atmospheric Chemistry and Physics, 2016,16(3):1433-1443.
[32]	Zhang X, Lin Y H, Surratt J D, et al. Sources, composition and absorption Angstrom exponent of light-absorbing organic components in aerosol extracts from the Los Angeles Basin[J]. Environmental Science and Technology, 2013,47(8):3685-93.
[33]	Kieber R J, Whitehead R F, Reid S N, et al. Chromophoric dissolved organic matter (CDOM) in rainwater, southeastern North Carolina, USA[J]. Journal of Atmospheric Chemistry, 2006,54(1):21-41.
[34]	Santos P S, Otero M, Duarte R M, et al. Spectroscopic characterization of dissolved organic matter isolated from rainwater[J]. Chemosphere 2009,74(8):1053-1061.
[35]	Santos P S, Santos E B, Duarte A C. First spectroscopic study on the structural features of dissolved organic matter isolated from rainwater in different seasons[J]. Science of the Total Environment, 2012,426:172-179.
[36]	Birdwell J E, Valsaraj K T. Characterization of dissolved organic matter in fogwater by excitation-emission matrix fluorescence spectroscopy[J]. Atmospheric Environment, 2010,44(27):3246-3253.
[37]	Qin J, Zhang L, Zhou X, et al. Fluorescence fingerprinting properties for exploring water-soluble organic compounds in PM2.5 in an industrial city of northwest China[J]. Atmospheric Environment, 2018, 184:203-211.
[38]	Zhang Y, Gao G, Shi K, et al. Absorption and fluorescence characteristics of rainwater CDOM and contribution to Lake Taihu, China[J]. Atmospheric Environment, 2014,98:483-491.
[39]	Matos J T, Freire S M, Duarte R M, et al. Natural organic matter in urban aerosols:Comparison between water and alkaline soluble components using excitation-emission matrix fluorescence spectroscopy and multiway data analysis[J]. Atmospheric Environment, 2015,102:1-10.
[40]	Santos P S, Otero M, Filipe O M, et al. Comparison between DAX-8 and C-18 solid phase extraction of rainwater dissolved organic matter[J]. Talanta, 2010,83(2):505-512.
[41]	Duarte R M, Pio C A, Duarte A C. Synchronous scan and excitation-emission matrix fluorescence spectroscopy of water-soluble organic compounds in atmospheric aerosols[J]. Journal of Atmospheric Chemistry, 2004,48(2):157-171.
[42]	Fu P, Kawamura K, Chen J, et al. Fluorescent water-soluble organic aerosols in the High Arctic atmosphere[J]. Scientific Reports, 2015, 5:9845.
[43]	McKnight D M, Boyer E W, Westerhoff P K, et al. pectrofluorometric characterization of dissolved organic matter for indication of precursor organic material and aromaticity[J]. Limnology and Oceanography, 2001,46(1):38-48.