Abstract:11 common substances, including straw, wood, coal, waste paper and waste plastics, were employed to simulate combustion in the laboratory and the methanol soluble organic matters (MSOM) in smoke were collected. The brown carbon in MSOM was characterized by UV-Vis and three-dimensional fluorescence spectroscopy (EEMs). Furthermore, non-negative matrix decomposition (NMF) was used to extract the characteristic excitation/emission spectra of main components of EEM, aiming to establish the basis of brown carbon traceability. The results show that the UV-vis spectra of straw and wood burning source brown carbon were similar with a shoulder peak at 265nm. The absorption of brown carbon from corrugated board and plastic combustion sources decreases singly with increasing wavelength. Due to the same basic components, the EEM of brown carbon corresponding to biomass and paperboard had similar profiles. NMF analysis showed three main fluorescent components in MSOM of biomass and paperboard, which were two humus C1, C2 and protein-like C3, respectively. The EEM of coal has a strong distribution in the long wave, which can be attributed to aromatic groups. From its EEM, the M1, M2 and M3 fluorophores can be decomposed and their positions are redshifted compared to those of biomass. According to fluorophore position and spectral signal profile, biomass and coal can be distinguished. Foam, plastic bag and plastic bottle are organic polymer materials and their EEM is quite different from that of biomass. The MSOM of foam and plastic bag contains four fluorescent components, while the MSOM of plastic bottle can only get two fluorophore groups with obvious characteristics.
邓汝乐, 高鹏, 贾松, 王雪飞. 燃烧生成棕色碳的三维荧光光谱分析[J]. 中国环境科学, 2022, 42(9): 3983-3990.
DENG Ru-le, GAO Peng, JIA Song, WANG Xue-fei. Comparisons of three - dimensional fluorescence spectra of brown carbon from combustion. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(9): 3983-3990.
Lin P, Fleming L T, Nizkorodov S A, et al. Comprehensive molecular characterization of atmospheric brown carbon by high resolution mass spectrometry with electrospray and atmospheric pressure photoionization [J]. Analytical Chemistry, 2018,90(21):12493-12502.
[2]
Wang Y J, Hu M, Li X, et al. Chemical Composition, Sources and Formation Mechanisms of Particulate Brown Carbon in the Atmosphere [J]. Progress in Chemistry, 2020,32(5):627-641.
[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(10):3131-3148.
[4]
Wu G M, Cong Z Y, Kang S C, et al. Brown carbon in the cryosphere: Current knowledge and perspective [J]. Advances in Climate Change Research, 2016,7(1/2):82-89.
[5]
Powelson M H, Espelien B M, Hawkins L N, et al. Brown carbon formation by aqueous-phase carbonyl compound reactions with amines and ammonium sulfate [J]. Environmental Science & Technology, 2014,48(2):985-993.
[6]
Gao Y, Wang Z X, Li Y B, et al. Aqueous brown carbon formation by aldehyde compounds reaction with Glycine/Ammonium sulfate [J]. Spectrochimica Acta Part a-Molecular and Biomolecular Spectroscopy, 2021,248:119230.
[7]
Gao Y, Zhang Y H. Optical properties investigation of the reactions between methylglyoxal and glycine/ammonium sulfate [J]. Spectrochimica Acta Part a-Molecular and Biomolecular Spectroscopy, 2019,215:112-121.
[8]
Hoffer A, Gelencser A, Guyon P, et al. Optical properties of humic- like substances (HULIS) in biomass-burning aerosols [J]. Atmospheric Chemistry and Physics, 2006,6:3563-3570.
[9]
Wu G M, Fu P Q, Ram K, et al. Fluorescence characteristics of water- soluble organic carbon in atmospheric aerosol [J]. Environmental Pollution, 2021,268:115906.
[10]
Xie C H, Xu W Q, Wang J F, et al. Vertical characterization of aerosol optical properties and brown carbon in winter in urban Beijing, China [J]. Atmospheric Chemistry and Physics, 2019,19(1):165-179.
[11]
韩 斌.聚氯乙烯等塑料废弃物热解特性及动力学研究 [D]. 天津:天津大学, 2012. Han B. Study on pyrolysis characteristics and kinetics of poly(vinyl chloride) and other plastics wastes [D]. Tianjin: Tianjin University, 2012.
[12]
江建方.城市生活垃圾外热式热解技术的研究 [D]. 武汉:华中科技大学, 2006. Jiang J F. Study on out heating pyrolysis technology of municipal solid waste [D]. Wuhan: Huazhong University of Science and Technology. 2006.
[13]
王 婷.北京大气有机气溶胶化学特征和光学性质研究 [D]. 广州:中国科学院大学(中国科学院广州地球化学研究所), 2021. Wang T. The chemical characteristics and optical properties of atmospheric organic aerosol in Beijing [D]. Guangzhou: Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, 2021.
[14]
Tang J, Li J, Su T, et al. Molecular compositions and optical properties of dissolved brown carbon in biomass burning, coal combustion, and vehicle emission aerosols illuminated by excitation-emission matrix spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry analysis [J]. Atmospheric Chemistry and Physics, 2020, 20(4):2513-2532.
[15]
Yan G, Kim G. Speciation and sources of brown carbon in precipitation at Seoul, Korea: Insights from excitation-emission matrix spectroscopy and carbon isotopic analysis [J]. Environmental Science & Technology, 2017,51(20):11580-11587.
[16]
陈 前.大气气相和颗粒相中棕碳化学组成及光学特性研究 [D]. 西安:陕西科技大学, 2021. Chen Q. Chemical composition and option properties of brown carbon in atmospheric gas and particulate phase[D]. Shaanxi University of Science and Technology, 2021.
[17]
白小梅,李悦昭,姚志鹏,等.三维荧光指纹谱在水体污染溯源中的应用进展 [J]. 环境科学与技术, 2020,43(1):172-180. Bai X M, Li Y Z, Yao Z P, et al. Application progress of three- dimensional excitation emission matrix fluorescence spectroscopy in source tracing of water pollution [J]. Environmental Science & Technology, 2020,43(1):172-180.
[18]
戴 源,谢继征,袁 静,等.三维荧光光谱技术结合线性支持向量算法在水体有机污染监测中的应用 [J]. 光谱学与光谱分析, 2021,41(9):2839-2845. Dai Y, Xie J Z, Yuan J, et al. Application of excitation-emission matrix (EEM) fluorescence combined with lindear SVM in organic pollution monitoring of water [J]. Spectroscopy and Spectral Analysis. 2021,41(9):2839-2845.
[19]
Boguta P, Pieczywek P M, Sokolowska Z. A comparative study of the application of fluorescence excitation-emission matrices combined with parallel factor analysis and nonnegative matrix factorization in the analysis of Zn complexation by humic acids [J]. Sensor, 2016, 16(10):1760.
[20]
孔 赟,朱 亮,吕梅乐,等.三维荧光光谱技术在水环境修复和废水处理中的应用 [J]. 生态环境学报, 2012,21(9):1647-1654. Kong Y, Zhu L, Lv M, et al. Research advances in water environment remediation and wastewater treatment based on three dimensional fluorescence spectroscopy technology [J]. Ecology and Environmental Sciences, 2012,21(9):1647-1654.
[21]
Coble P G. Characterization of marine and terrestrial DOM in seawater using excitation emission matrix spectroscopy [J]. Marine Chemistry, 1996,51(4):325-346.
[22]
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.
[23]
范行军,操 涛,余旭芳,等.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 X J, Cao T, Yu X F, et al. Emission characteristics and optical properties of extractable brown carbon from residential wood combustion [J]. China Environmental Science, 2019,39(8):3215-3224.
[24]
Lee D D, Seung H S. Learning the parts of objects by non-negative matrix factorization [J]. Nature, 1999,401(6755):788-791.
[25]
余肖玲.非负矩阵分解理论及其在高光谱解混中的应用 [D]. 成都:成都理工大学, 2015. Yu X L. The theory of Non negative matrix factorization and its application in the highspectrual unmixing [D]. Chengdu: Chengdu University of Technology, 2015.
[26]
Debas H T, Soon-Shiong P, Mckenzie A D, et al. Use of secretin in the roentgenologic and biochemical diagnosis of duodenal gastrinoma [J]. The American Journal of Surery, 1983,145(3):408-411.
[27]
贾 旭,孙福明,李豪杰,等.具有普适性的改进非负矩阵分解图像特征提取方法 [J]. 计算机应用, 2018,38(1):233-237,254. Jia X, Sun F M, Li H J, et al. Image feature extraction method based on improved nonnegative matrix factorization with universality [J]. Journal of Computer Applications, 2018,38(1):233-237,254.
[28]
张 翼,王丽君,庞宝川.基于非负矩阵分解的病理图像染色分离方法 [J]. 信息技术, 2018,42(6):12-16. Zhang Y, Wang L J, Pang B C. The method of pathological image dyeing separation based on non-negative matrix factorization [J]. Imformation Technology, 2018,42(6):12-16.
[29]
秦楚雄,张连海.基于非负矩阵分解的语音深层低维特征提取方法 [J]. 数据采集与处理, 2017,145(5):921-930. Qin C X, Zhang L H. Nonnegative matrix factorization based deep low-dimensional feature extraction approach for speech recognition [J]. Journal of Data Acquisition and Processing, 2017,145(5):921-930.
[30]
李勇智,杨静宇.基于非负矩阵分解新的人脸识别方法 [J]. 系统仿真学报, 2008,158(1):111-116. Li Z Y, Yang J Y. Novel methods of face recognition based on non- negative matrix factorization [J]. Journal of System Simulation, 2008, 158(1):111-116.
[31]
Yang Q, Zhou H W, Bartocci P, et al. Prospective contributions of biomass pyrolysis to China's 2050 carbon reduction and renewable energy goals [J]. Nature Communications, 2021,12(1):1698.
[32]
巩志强.生物质直接再燃脱硝特性试验研究 [D]. 济南:山东大学, 2008. Gong Z Q. Experimental study on performance of biomass reburning for NOx reduction [D]. Jinan: Shangdong University, 2008.
[33]
张震娇,张久东,刘彩红,等.西北干旱地区边际土地高抗逆纤维类能源植物的筛选与初探 [J]. 中国农业文摘-农业工程, 2017,29(1): 15-20. Zhang Z J, Zhang J D, Liu C H, et al. Screening and exploration energy plants with high resistance in northwest arid region [J]. Agricultural Science and Engineering in China, 2017,29(1):15-20.
[34]
田 红,廖正祝.农业生物质燃烧特性及燃烧动力学 [J]. 农业工程学报, 2013,29(10):203-212. Tian H, Liao Z Z. Combustion characteristics and combustion kinetics of agriculture biomass [J]. Transactions of the Chinese Society of Agricultural Engineering, 2013,29(10):203-212.
[35]
李美菊.家用燃煤燃烧排放颗粒物中棕色碳的化学性质与光学特征研究 [D]. 北京:中国科学院大学(中国科学院广州地球化学研究所), 2018. Li M J. Chemical and light absorption properties of brown carbon emitted from residential coal combustion in China [D]. Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, 2018.
[36]
Tian J, Ni H Y, Cao J J, et al. Characteristics of carbonaceous particles from residential coal combustion and agricultural biomass burning in China [J]. Atmospheric Pollution Research, 2017,8(3):521-527.
[37]
Booksh K S, Muroski A R, Myrick M L. Single measurement excitation/emission matrix spectrofluorometer for determination of hydrocarbons in ocean water .2. Calibration and quantitation of naphthalene and styrene [J]. Analytical Chemistry, 1996,68(20):3539- 3544.
[38]
顾乾恒.EEMs-PARAFAC法分析环境中DOM常见组分简述 [J]. 广东化工, 2021,48(16):87-88,76. Gu Q H. Common components of DOM in the environment analyzed by EEMS-PARAFAC method [J]. Guangdong Chemical Industry 2021,48(16):87-88,76.
[39]
吴正华,钱益武,刘小勇,等.基于水质三维荧光技术的城市河流水质污染分析 [J]. 水资源与水工程学报, 2020,31(6):41-46. Wu Z H, Qian Y W, Liu X Y, et al. Analysis of urban river water pollution based on three-dimensional fluorescence spectrometry of water quality [J]. Journal of Water Resources & Water Engineering, 2020,31(6):41-46.
[40]
林绍霞,肖致强,张转铃,等.贵州草海水体溶解性有机物的荧光光谱特征及来源解析 [J]. 中国环境科学, 2021,41(3):1325-1335. Lin S X, Xiao Z Q, Zhang Z L, et al. Fluorescence spectral characteristics and source apportionment of dissolved organic matters in water of Caohai Lake, Guizhou Province [J]. China Environmental Science, 2021,41(3):1325-1335.
[41]
Wu G M, Ram K, Fu P Q, et al. Water-soluble brown carbon in atmospheric aerosols from godavari (Nepal), a regional representative of South Asia [J]. Environmental Science & Technology, 2019,53(7): 3471-3479.
[42]
吕伟伟,姚 昕,张保华,等.太湖颗粒态有机质的荧光特征及环境指示意义 [J]. 环境科学, 2018,39(5):2056-2066. Lv W W, Yao X, Zhang B H, et al. Fluorescent characteristics and environmental significance of particulate organic matter in Lake Taihu,China [J]. Environmental Science, 2018,39(5):2056-2066.
[43]
Wu G M, Wan X, Ram K, et al. Light absorption, fluorescence properties and sources of brown carbon aerosols in the Southeast Tibetan Plateau [J]. Environmental Pollution, 2020,257:113616.
王 翔,赵南京,殷高方,等.基于反向传播神经网络的激光诱导荧光光谱塑料分类识别方法研究 [J]. 光谱学与光谱分析, 2019,39(10): 3136-3141. Wang X, Zhao N J, Yin G F, et al. Classification and identification of plastic with laser-induced fluorescence spectroscopy based on back propagation neural network model [J]. Spectroscopy and Spectral Analysis, 2019,39(10):3136-3141.
[46]
Jin Z C, Yin L, Chen D Z, et al. Co-pyrolysis characteristics of typical components of waste plastics in a falling film pyrolysis reactor [J]. Chinese Journal of Chemical Engineering, 2018,26(10):2176-2184.
[47]
Wang J, Liu X H, Liu G N, et al. Size effect of polystyrene microplastics on sorption of phenanthrene and nitrobenzene [J]. Ecotoxicology and Environmental Safety, 2019,173:331-338.