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薪柴燃烧溶解性棕色碳排放特征及光学性质
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.
作者姓名:范行军  操涛  余旭芳  宋建中  王艳  肖新  谢越  李飞跃
作者单位:1. 安徽科技学院资源与环境学院, 安徽 凤阳 233100;2. 中国科学院广州地球化学研究所有机地球化学国家重点实验室, 广东 广州 510640;3. 中国科学院大学, 北京 100049
基金项目: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)
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(HULISWS)、碱溶性有机物(ASOM)和碱溶性类腐殖质(HULISAS)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BrCT(WSOM+ASOM)占烟气PM2.5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BrCT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βα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.

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  
收稿时间:2019-01-28

Emission characteristics and optical properties of extractable brown carbon from residential wood combustion
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[J].China Environmental Science,2019,39(8):3215-3224.
Authors:FAN Xing-jun  CAO Tao  YU Xu-fang  SONG Jian-zhong  WANG Yan  XIAO Xin  XIE Yue  LI Fei-yue
Institution:1. College of Resources and Environment, Anhui Science and Technology University, Fengyang 233100, China;2. State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China;3. University of Chinese Academy of Sciences, Beijing 100049, China
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 (HULISWS), alkaline-soluble organic matters (ASOM), alkaline-soluble HULIS (HULISAS), emitted from household residential wood combustion. The results showed that residential wood combustion emitted large amounts of BrC. Among them, BrCT (WSOM + ASOM) were observed to make up 46%~56% of total smoke PM2.5 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 BrCT. 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.
Keywords:residential wood combustion  brown carbon  emission characteristics  light absorption  fluorescence spectral properties  
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