南京大学学报(自然科学版) ›› 2021, Vol. 57 ›› Issue (3): 356363.doi: 10.13232/j.cnki.jnju.2021.03.002
摘要:
有机化合物在溶解性有机质(Dissolved Organic Matter,DOM)上的吸附行为显著影响其环境归趋和生物有效性.以标化的DOM紫外?可见光谱和有机化合物的正辛醇?水分配系数为特征,运用随机森林算法,建立有机碳标化分配系数(KOC)的预测模型.结果显示,随机森林模型在全部来源DOM上的预测精度显著高于目前普遍使用的线性自由能模型,但略低于两相体系模型.随机森林模型对土壤和泥炭来源的DOM吸附预测精度显著优于其他模型,说明随机森林模型具有很好的适用性.根据随机森林模型输出的特征重要性,发现模型学习到了表征DOM分子量大小、腐殖化程度以及苯环上取代基类型的光谱特征.通过特征选择,发现模型使用少数重要性较高的特征可以达到使用全谱的效果,即使在只选取两个波长时,预测精度依然显著优于线性自由能模型.由于DOM的紫外?可见光谱可原位实时分析,基于紫外?可见光谱和机器学习方法的预测模型未来可进行原位及高通量KOC时空规律解析,从而实现更准确更精细的风险评估与管理.
中图分类号:
1 | Chiou C T,Peters L J,Freed V H. A physical concept of soil?water equilibria for nonionic organic compounds. Science,1979,206 (4420):831-832. |
2 | Luthy R G,Aiken G R,Brusseau M L,et al. Sequestration of hydrophobic organic contaminants by geosorbents. Environmental Science & Technology,1997,31 (12):3341-3347. |
3 | Bronner G,Goss K U. Predicting sorption of pesticides and other multifunctional organic chemicals to soil organic carbon. Environmental Science & Technology,2011,45 (4):1313-1319. |
4 | Chiou C T,Porter P E,Schmedding D W. Partition equilibriums of nonionic organic compounds between soil organic matter and water. Environmental Science & Technology,1983,17 (4):227-231. |
5 | Endo S,Goss K U. Applications of polyparameter linear free energy relationships in environmental chemistry. Environmental Science & Technology,2014,48 (21):12477-12491. |
6 | Goss K U,Schwarzenbach R P. Linear free energy relationships used to evaluate equilibrium partitioning of organic compounds. Environmental Science & Technology,2001,35 (1):1-9. |
7 | Nguyen T H,Goss K U,Ball W P. Polyparameter linear free energy relationships for estimating the equilibrium partition of organic compounds between water and the natural organic matter in soils and sediments. Environmental Science & Technology,2005,39 (4):913-924. |
8 | Zhu D Q,Pignatello J J. A concentration?dependent multi?term linear free energy relationship for sorption of organic compounds to soils based on the hexadecane dilute?solution reference state. Environmental Science & Technology,2005,39 (22):8817-8828. |
9 | Fu H Y,Liu K,Alvarez P J J,et al. Quantifying hydrophobicity of natural organic matter using partition coefficients in aqueous two?phase systems. Chemosphere,2019,218:922-929. |
10 | Liu K,Fu H Y,Zhu D Q,et al. Prediction of apolar compound sorption to aquatic natural organic matter accounting for natural organic matter hydrophobicity using aqueous two?phase systems. Environmental Science & Technology,2019,53 (14):8127-8135. |
11 | Peuravuori J,Pihlaja K. Molecular size distribution and spectroscopic properties of aquatic humic substances. Analytica Chimica Acta,1997,337 (2):133-149. |
12 | Helms J R,Stubbins A,Ritchie J D,et al. Absorption spectral slopes and slope ratios as indicators of molecular weight,source,and photobleaching of chromophoric dissolved organic matter. Limnology and Oceanography,2008,53 (3):955-969. |
13 | Chin Y P,Aiken G,O'Loughlin E. Molecular weight,polydispersity,and spectroscopic properties of aquatic humic substances. Environmental Science & Technology,1994,28 (11):1853-1858. |
14 | Breiman L. Random forests. Machine Learning,2001,45 (1):5-32. |
15 | Breiman L. Bagging predictors. Machine Learning,1996,24 (2):123-140. |
16 | Sun H Y,Shi X,Mao J D,et al. Tetracycline sorption to coal and soil humic acids:An examination of humic structural heterogeneity. Environmental Toxicology and Chemistry,2010,29(9):1934-1942. |
17 | Korshin G V,Li C W,Benjamin M M. Monitoring the properties of natural organic matter through UV spectroscopy:A consistent theory. Water Research,1997,31 (7):1787-1795. |
18 | Chin Y P,Aiken G R,Danielsen K M. Binding of pyrene to aquatic and commercial humic substances:The role of molecular weight and aromaticity. Environmental Science & Technology,1997,31 (6):1630-1635. |
19 | Fu H Y,Wei C H,Qu X L,et al. Strong binding of apolar hydrophobic organic contaminants by dissolved black carbon released from biochar:A mechanism of pseudomicelle partition and environmental implications. Environmental Pollution,2018 (232):402-410. |
20 | Liu K,Kong L R,Wang J X,et al. Two?phase system model to assess hydrophobic organic compound sorption to dissolved organic matter. Environmental Science & Technology,2020,54 (19):12173-12180. |
21 | Yao X,Zhang Y L,Zhu G W,et al. Resolving the variability of CDOM fluorescence to differentiate the sources and fate of DOM in Lake Taihu and its tributaries. Chemosphere,2011,82 (2):145-155. |
22 | Abraham M H,Doherty R M,Kamlet M J,et al. Linear solvation energy relationships. Part38. An analysis of the use of solvent parameters in the correlation of rate constants,with special reference to the solvolysis of t?butyl chloride. Journal of the Chemical Society,Perkin Transactions,1987,2 (8):1097-1101. |
23 | Abraham M H,Doherty R M,Kamlet M J,et al. Linear solvation energy relationships. Part37. An analysis of contributions of dipolarity?polarisability,nucleophilic assistance,electrophilic assistance,and cavity terms to solvent effects on t?butyl halide solvolysis rates. Journal of the Chemical Society,Perkin Transactions,1987,2 (7):913-920. |
24 | Bergstra J,Bardenet R,Bengio Y,et al. Algorithms for hyper?parameter optimization∥Proceedings of the 24th International Conference on Neural Information Processing Systems. Red Hook,NY,USA:Curran Associates Inc.,2011:2546-2554. |
25 | Hutter F,Hoos H H,Leyton?Brown K. Sequential model?based optimization for general algorithm configuration∥Learning and Intelligent Optimization. Springer Berlin Heidelberg,2011:507-523. |
26 | Wang L Y,Wu F C,Zhang R Y,et al. Characterization of dissolved organic matter fractions from Lake Hongfeng,Southwestern China Plateau. Journal of Environmental Sciences,2009,21 (5):581-588. |
27 | Huo S L,Xi B D,Zan F Y,et al. Dissolved organic matter in digested piggery wastewater from combined treatment process. Desalination and Water Treatment,2013,51 (10-12):2351-2361. |
[1] | 曹欣怡,李鹤,王蔚. 基于语料库的语音情感识别的性别差异研究[J]. 南京大学学报(自然科学版), 2019, 55(5): 758-764. |
[2] | 王鹏,林志斌. 基于响度级、耳间互相关系数和中心频率的主观声场宽度预测模型[J]. 南京大学学报(自然科学版), 2019, 55(5): 804-812. |
[3] | 阚 威, 李 云. 基于LSTM的脑电情绪识别模型[J]. 南京大学学报(自然科学版), 2019, 55(1): 110-116. |
[4] | 王卓君,申德荣*,聂铁铮,寇 月,于 戈. UCM-PPM:基于用户分级的多参量Web预测模型[J]. 南京大学学报(自然科学版), 2018, 54(1): 85-. |
[5] | 朱亚奇1,邓维斌1 ,2*. 一种基于不平衡数据的聚类抽样方法[J]. 南京大学学报(自然科学版), 2015, 51(2): 421-429. |
[6] | 朱亚奇1,邓维斌1,2*. 一种基于不平衡数据的聚类抽样方法[J]. 南京大学学报(自然科学版), 2015, 51(2): 421-429. |
[7] | 刘紫赞,沈勇,王思理,沈坚 . 用客观测量数据预测微型扬声器感知音质的复回归模型[J]. 南京大学学报(自然科学版), 2012, 48(5): 648-653. |
|