中国环境科学
 
 
中国环境科学  2022, Vol. 42 Issue (8): 3483-3491    DOI:
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生物质燃烧源类腐殖质的臭氧老化特征
操涛1,2,4, 宋建中1,2, 范行军1,3
1. 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;
2. 中国科学院深地科学卓越创新中心, 广东 广州 510640;
3. 安徽科技学院资源与环境学院, 安徽 蚌埠 233100;
4. 中国科学院大学, 北京 100049
Changes in optical properties and chemical functional groups of humic substances emitted from biomass combustion with O3 oxidation
CAO Tao1,2,4, SONG Jian-zhong1,2, FAN Xing-jun1,3
1. State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China;
2. CAS Center for Excellence in Deep Earth Science, Guangzhou 510640, China;
3. College of Resource and Environment, Anhui Science and Technology University, Bengbu 233100, China;
4. University of Chinese Academy of Sciences, Beijing 100049, China

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摘要 针对生物质燃烧排放类腐殖质(BC-HULIS)的臭氧(O3)氧化开展模拟研究,利用总有机碳分析仪(TOC)、紫外-可见吸收光谱(UV-vis)、荧光激发发射矩阵光谱结合平行因子分析(EEM-PARAFAC)以及傅里叶变换红外光谱(FTIR)表征老化前后HULIS的光学性质和化学结构变化.研究表明,经臭氧氧化后BC-HULIS占相应的水溶性有机碳(WSOC)的比例降低,表明部分HULIS发生降解生成水溶性小分子化合物.此外经O3老化后,HULIS的质量吸收指数(MAE365)和芳香性指数(SUVA254)分别从1.8~2.7和4.2~5.0m2/gC下降到1.1~1.3和3.7~4.1m2/gC,表明老化后HULIS的吸光能力和芳香度均呈现降低.EEM-PARAFAC解析结果显示,BB-HULIS中荧光发色团主要由类蛋白荧光组分(C2)和类腐殖质荧光组分(C1、C3、C4)组成.O3老化后,BB-HULIS的总荧光强度显著降低,两种性质的荧光组分相对含量和荧光参数发生显著变化,如老化后HULIS中类腐殖质荧光组分的相对含量和腐质化指数(HIX)均显著高于老化前样品,表明老化过程发生类蛋白的降解和类腐殖质的聚合.另外,FTIR分析结果显示O3老化后含氧官能团含量显著增强,表明了O3老化对HULIS官能团的影响.
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操涛
宋建中
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关键词 生物质燃烧类腐殖质臭氧氧化光学性质化学结构    
Abstract:Biomass combustion (BC) is an important source of humic-like substances (HULIS) in atmospheric aerosol, and the oxidation process has a significant impact on the optical properties and chemical structures of BC-HULIS. This study focused on the changes in primary BB-HULIS due to ozone (O3) oxidation and the optical properties and chemical structure of HULIS before and after oxidation were characterized with the total organic carbon (TOC) analyzer, UV-Vis spectroscopy, Excitation-Emission Matrix coupled with parallel factor analysis (EEM-PARAFAC) and Fourier transform infrared spectroscopy (FTIR). The results showed that the relative contents of HULIS in the corresponding water-soluble organic carbon (WSOC) decreased with O3 oxidation, suggesting the transformation of HULIS into water-soluble low molecular weight compounds. Furthermore, mass absorption efficiency (MAE365) and aromatic index (SUVA254) of HULIS decreased from 1.8~2.7m2/gC and 4.2~5.0m2/gC to 1.1~1.3m2/gC and 3.7~4.1m2/gC, respectively, indicating that both the absorption capacity and aromaticity of HULIS declined with O3 oxidation. The fluorescent components in BC-HULIS were mainly composed of protein-like compounds (C2) and humic-like substances (C1, C3, C4). After O3 oxidation, the total fluorescence intensities of BC-HULIS weakened greatly, and the relative contribution of two types of fluorophores and fluorescence index were all significantly changed. For instances, the relative contents of humic-like components and the humidification index (HIX) of BC-HULIS after O3 oxidation were obviously higher than those before O3 oxidation, suggesting the degradation of protein-like compounds and the aggregation of humic-like substances during the O3 oxidation process. In addition, FTIR results showed that the oxygen-containing functional groups were markedly enhanced after O3 oxidation, indicating effects of O3 oxidation on the chemical functional groups of BC-HULIS.
Key wordsbiomass burning    HULIS    ozone oxidation    optical properties    chemical structure   
收稿日期: 2022-01-17     
PACS: X513  
基金资助:国家自然科学基金资助项目(41977188);有机地球化学国家重点实验室开放基金资助项目(SKLOG202101);安徽省自然科学基金资助项目(2108085MD140)
通讯作者: 范行军,副教授,fanxj@ahstu.edu.cn     E-mail: fanxj@ahstu.edu.cn
作者简介: 操涛(1995-)男,安徽安庆人,中国科学院广州地球化学研究所博士研究生,主要从事生物质和煤燃烧排放棕色碳等吸光性物质的研究.发表论文1篇.
引用本文:   
操涛, 宋建中, 范行军. 生物质燃烧源类腐殖质的臭氧老化特征[J]. 中国环境科学, 2022, 42(8): 3483-3491. CAO Tao, SONG Jian-zhong, FAN Xing-jun. Changes in optical properties and chemical functional groups of humic substances emitted from biomass combustion with O3 oxidation. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(8): 3483-3491.
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