大气污染物监测数据不确定度评估方法体系建立及其对PMF源解析的影响分析
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摘要
目前,正定矩阵因子法(PMF)在大气污染物来源解析中得到了广泛应用,而监测数据不确定度评估是PMF源解析的重要内容之一.当前绝大部分研究采用的数据不确定度仅通过借鉴前人的方法简单计算而得,缺乏对计算方法的合理性和适用性进行评估.本研究通过3种常用的不确定度算法交互应用建立了一套有效评估不确定度的方法体系.通过对香港荃湾站点1998—2008年PM_(10)组分监测数据进行源解析并与平行采样数据源解析结果进行对比,对该方法体系的合理性进行了验证.结果发现,应用该方法体系可以将某些常规方法无法分离的因子进一步分解,得到的源解析结果的残差值甚至小于平行采样方法解析结果的残差值,得到的因子贡献率均处于常规方法得出的因子贡献率之间.这些均表明了该方法体系所得源解析结果的可靠性和全面性.因此,本研究建立的评估不确定度的方法体系具有较强的可行性,对确保源解析结果的准确性有重要意义.
Positive matrix factorization(PMF) has been applied extensively in source apportionment of atmospheric pollutants. Data uncertainty is one of the most important input information for PMF analysis. Currently, data uncertainty is calculated by some simple formulae referenced from previous studies, lacking evaluation of their reasonableness and applicability. In this study, we develop an uncertainty assessment framework(UAF) by utilizing three common uncertainty calculation algorithms. The effectiveness of this UAF is assessed by comparing with the source apportionment results on parallel measurement of PM_(10) compositions at Tsuen Wan station in Hong Kong during 1998—2008. It is found that applying UAF could further decompose some factors which couldn′t by traditional methods. The derived scaled residuals are even smaller than those from source apportionment on parallel measurement. Source contributions derived by UAF are well in between those from traditional methods. All above indicates the reliability and completeness of source apportionment by UAF. It is thus concluded that this UAF has great applicability and usefulness in ensuring the accuracy of source apportionment results.
Positive matrix factorization(PMF) has been applied extensively in source apportionment of atmospheric pollutants. Data uncertainty is one of the most important input information for PMF analysis. Currently, data uncertainty is calculated by some simple formulae referenced from previous studies, lacking evaluation of their reasonableness and applicability. In this study, we develop an uncertainty assessment framework(UAF) by utilizing three common uncertainty calculation algorithms. The effectiveness of this UAF is assessed by comparing with the source apportionment results on parallel measurement of PM_(10) compositions at Tsuen Wan station in Hong Kong during 1998—2008. It is found that applying UAF could further decompose some factors which couldn′t by traditional methods. The derived scaled residuals are even smaller than those from source apportionment on parallel measurement. Source contributions derived by UAF are well in between those from traditional methods. All above indicates the reliability and completeness of source apportionment by UAF. It is thus concluded that this UAF has great applicability and usefulness in ensuring the accuracy of source apportionment results.
引文
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边璐,李田,侯娟.2013.PMF和PCA/MLR法解析上海市高架道路地表径流中多环芳烃的来源[J].环境科学, 34(10):3840-3846
Cheng Y,Lee S C,Ho K F,et al.2010.Chemically-speciated on-road PM2.5 motor vehicle emission factors in Hong Kong[J].Science of the Total Environment, 408(7):1621-1627
Cai C,Geng F,Tie X,et al.2010.Characteristics and source apportionment of VOCs measured in Shanghai,China[J].Atmospheric Environment,44(38):5005-5014
US Environmental Protection Agency. EPA Positive Matrix Factorization 5.0 Fundamentals and User Guide[OL]. 2018-01-06.https://www.epa.gov/sites/production/files/2015-02/documents/pmf_5.0_user_guide.pdf.
Fang Y,Chen Y,Tian C,et al.2016.Application of PMF receptor model merging with PAHs signatures for source apportionment of black carbon in the continental shelf surface sediments of the Bohai and Yellow Seas,China[J].Journal of Geophysical Research - Oceans,121(2):1346-1359
Friend A J,Ayoko G A,Guo H.2011.Multi-criteria ranking and receptor modelling of airborne fine particles at three sites in the Pearl River Delta region of China [J].Science of the Total Environment,409(4):719-737
Gao B,Guo H,Wang X M,et al.2013.Tracer-based source apportionment of polycyclic aromatic hydrocarbons in PM2.5,in Guangzhou,southern China,using positive matrix factorization (PMF) [J].Environmental Science - & Pollution Research International,20(4):2398-2409
Gao B,Wang X M,Zhao X Y,et al.2015.Source apportionment of atmospheric PAHs and their toxicity using PMF: Impact of gas/particle partitioning [J].Atmospheric Environment,103:114-120
Guo H,Ding A J,So K L,et al.2009.Receptor modeling of source apportionment of Hong Kong aerosols and the implication of urban and regional contribution [J].Atmospheric Environment,43(6):1159-1169
环境保护部.2013.大气颗粒物来源解析技术指南 (试行)[OL].2018-01-08.http://www.zhb.gov.cn/gkml/hbb/bwj/201308/W020130820340683623095.pdf
Huang R J,Zhang Y,Bozzetti C,et al.2014.High secondary aerosol contribution to particulate pollution during haze events in China[J].Nature,514(7521):218-222
Huang S,Rahn K A,Arimoto R.2008.Testing and optimizing two factor-analysis techniques on aerosol at Narragansett,Rhode Island[J].Atmospheric Environment,33(14):2169-2185
Hyslop N P,White W H.An evaluation of interagency monitoring of protected visual environments (IMPROVE) collocated precision and uncertainty estimates[J].Atmospheric Environment,42(11):2691-2705
Ito K,Xue N,Thurston G.2004.Spatial variation of PM2.5,chemical species and source-apportioned mass concentrations in New York City[J].Atmospheric Environment,38(31):5269-5282
Jiang Y,Liu P.2014.Feature extraction for identification of drug and explosive concealed by body packing based on positive matrix factorization[J].Measurement,47(1):193-199
梁林林,Guenter,Engling,段凤魁,等.2015.北京市大气气溶胶中糖类化合物的组成及来源[J].环境科学,36(11):3935-3942
Liu P,Li Z,Li B,et al.2013.The analysis of time-resolved optical waveguide absorption spectroscopy based on positive matrix factorization[J].Journal of Colloid & Interface Science,403:134
刘胜林.2003.误差分析与测量不确定度评定[M].北京:中国计量出版社
Paatero P,Tapper U.1994.Positive matrix factorization: A non-negative factor model with optimal utilization of error estimates of data values[J].Environmetrics,5(2):111-126
Paatero P.1997.A weighted non-negative least squares algorithm for three-way ‘PARAFAC’ factor analysis[J].Chemometrics & Intelligent Laboratory Systems,38(2):223-242
Polissar A V,Hopke P K,Paatero P,et al.1998.Atmospheric aerosol over Alaska: 2.Elemental composition and sources[J].Journal of Geophysical Research - Atmospheres,103(D15):19045-19057
Prendes P,Andrade J M,López-MahíA P,et al.1999.Source apportionment of inorganic ions in airborne urban particles from Coruňa city(N.W.of Spain)using positive matrix factorization[J].Talanta,49(1):165-178
Tan J H,Duan J C,Chai F H,et al.2014.Source apportionment of size segregated fine/ultrafine particle by PMF in Beijing[J].Atmospheric Research,139(6):90-100
Tao J,Zhang L,Zhang R,et al. 2016.Uncertainty assessment of source attribution of PM2.5 and its water-soluble organic carbon content using different biomass burning tracers in positive matrix factorization analysis-a case study in Beijing,China [J].Science of the Total Environment,543(Pt A):326-335
Tian S L,Pan Y P,Wang Y S.2017.Size-resolved source apportionment of particulate matter in urban Beijing during haze and non-haze episodes[J].Atmospheric Chemistry & Physics Discussions,16(1):9405-9443
Wang Q,He X,Huang X H H,et al.Impact of secondary organic aerosol tracers on tracer-based source apportionment of organic carbon and PM2.5: A case study in the Pearl River Delta,China[J] ACS Earth Space Chemistry,1:562-571
Wang F,Lin T,Feng J,et al.2015.Source apportionment of polycyclic aromatic hydrocarbons in PM2.5 using positive matrix factorization modeling in Shanghai,China[J].Environmental Science Processes & Impacts,17(1):197-205
Wang Y,Li L,Chen C,et al.2014.Source apportionment of fine particulate matter during autumn haze episodes in Shanghai,China [J].Journal of Geophysical Research Atmospheres,119(4):1903-1914
王琴,张大伟,刘保献,等.2015.基于PMF模型的北京市PM2.5来源的时空分布特征[J].中国环境科学,35(10):2917-2924
Xie Y L,Hopke P K,Paatero P,et al.1999.Identification of source nature and seasonal variations of Arctic aerosol by the multilinear engine[J].Atmospheric Environment,33(16):2549-2562
Yao L,Yang L,Yuan Q,et al.2016.Sources apportionment of PM2.5,in a background site in the North China Plain[J].Science of the Total Environment,541:590-598
Yu J Z,Lau A K H,Louie K K,et al.2004.Abundance and seasonal characteristics of elemental and organic carbon in Hong Kong PM10[J].Atmospheric Environment,38(10):1511-1521
Yuan Z,Lau A K H,Zhang H,et al.2006.Identification and spatiotemporal variations of dominant PM10,sources over Hong Kong [J].Atmospheric Environment,40(10):1803-1815
Yuan Z,Yadav V,Turner J R,et al.2013.Long-term trends of ambient particulate matter emission source contributions and the accountability of control strategies in Hong Kong over 1998—2008[J].Atmospheric Environment,76(3):21-31
Zhang Y,Jing C,Wang S,et al.2017.Review of receptor-based source apportionment research of fine particulate matter and its challenges in China[J].Science of the Total Environment,586:917-929
Zhang R,Jing J,Tao J,et al.2013.Chemical characterization and source apportionment of PM2.5 in Beijing: seasonal perspective[J].Atmospheric Chemistry & Physics,13(14):7053-7074
Zíková N,Wang Y,Yang F,et al. 2016.On the source contribution to Beijing PM2.5 concentrations [J].Atmospheric Environment,134:84-95
郑君瑜,王水胜,黄志炯,等.2013.区域高分辨率大气排放源清单建立的技术方法与应用[M].北京:科学出版社
张延君,郑玫,蔡靖,等.2015.PM2.5源解析方法的比较与评述[J].科学通报,(2):109-121
边璐,李田,侯娟.2013.PMF和PCA/MLR法解析上海市高架道路地表径流中多环芳烃的来源[J].环境科学, 34(10):3840-3846
Cheng Y,Lee S C,Ho K F,et al.2010.Chemically-speciated on-road PM2.5 motor vehicle emission factors in Hong Kong[J].Science of the Total Environment, 408(7):1621-1627
Cai C,Geng F,Tie X,et al.2010.Characteristics and source apportionment of VOCs measured in Shanghai,China[J].Atmospheric Environment,44(38):5005-5014
US Environmental Protection Agency. EPA Positive Matrix Factorization 5.0 Fundamentals and User Guide[OL]. 2018-01-06.https://www.epa.gov/sites/production/files/2015-02/documents/pmf_5.0_user_guide.pdf.
Fang Y,Chen Y,Tian C,et al.2016.Application of PMF receptor model merging with PAHs signatures for source apportionment of black carbon in the continental shelf surface sediments of the Bohai and Yellow Seas,China[J].Journal of Geophysical Research - Oceans,121(2):1346-1359
Friend A J,Ayoko G A,Guo H.2011.Multi-criteria ranking and receptor modelling of airborne fine particles at three sites in the Pearl River Delta region of China [J].Science of the Total Environment,409(4):719-737
Gao B,Guo H,Wang X M,et al.2013.Tracer-based source apportionment of polycyclic aromatic hydrocarbons in PM2.5,in Guangzhou,southern China,using positive matrix factorization (PMF) [J].Environmental Science - & Pollution Research International,20(4):2398-2409
Gao B,Wang X M,Zhao X Y,et al.2015.Source apportionment of atmospheric PAHs and their toxicity using PMF: Impact of gas/particle partitioning [J].Atmospheric Environment,103:114-120
Guo H,Ding A J,So K L,et al.2009.Receptor modeling of source apportionment of Hong Kong aerosols and the implication of urban and regional contribution [J].Atmospheric Environment,43(6):1159-1169
环境保护部.2013.大气颗粒物来源解析技术指南 (试行)[OL].2018-01-08.http://www.zhb.gov.cn/gkml/hbb/bwj/201308/W020130820340683623095.pdf
Huang R J,Zhang Y,Bozzetti C,et al.2014.High secondary aerosol contribution to particulate pollution during haze events in China[J].Nature,514(7521):218-222
Huang S,Rahn K A,Arimoto R.2008.Testing and optimizing two factor-analysis techniques on aerosol at Narragansett,Rhode Island[J].Atmospheric Environment,33(14):2169-2185
Hyslop N P,White W H.An evaluation of interagency monitoring of protected visual environments (IMPROVE) collocated precision and uncertainty estimates[J].Atmospheric Environment,42(11):2691-2705
Ito K,Xue N,Thurston G.2004.Spatial variation of PM2.5,chemical species and source-apportioned mass concentrations in New York City[J].Atmospheric Environment,38(31):5269-5282
Jiang Y,Liu P.2014.Feature extraction for identification of drug and explosive concealed by body packing based on positive matrix factorization[J].Measurement,47(1):193-199
梁林林,Guenter,Engling,段凤魁,等.2015.北京市大气气溶胶中糖类化合物的组成及来源[J].环境科学,36(11):3935-3942
Liu P,Li Z,Li B,et al.2013.The analysis of time-resolved optical waveguide absorption spectroscopy based on positive matrix factorization[J].Journal of Colloid & Interface Science,403:134
刘胜林.2003.误差分析与测量不确定度评定[M].北京:中国计量出版社
Paatero P,Tapper U.1994.Positive matrix factorization: A non-negative factor model with optimal utilization of error estimates of data values[J].Environmetrics,5(2):111-126
Paatero P.1997.A weighted non-negative least squares algorithm for three-way ‘PARAFAC’ factor analysis[J].Chemometrics & Intelligent Laboratory Systems,38(2):223-242
Polissar A V,Hopke P K,Paatero P,et al.1998.Atmospheric aerosol over Alaska: 2.Elemental composition and sources[J].Journal of Geophysical Research - Atmospheres,103(D15):19045-19057
Prendes P,Andrade J M,López-MahíA P,et al.1999.Source apportionment of inorganic ions in airborne urban particles from Coruňa city(N.W.of Spain)using positive matrix factorization[J].Talanta,49(1):165-178
Tan J H,Duan J C,Chai F H,et al.2014.Source apportionment of size segregated fine/ultrafine particle by PMF in Beijing[J].Atmospheric Research,139(6):90-100
Tao J,Zhang L,Zhang R,et al. 2016.Uncertainty assessment of source attribution of PM2.5 and its water-soluble organic carbon content using different biomass burning tracers in positive matrix factorization analysis-a case study in Beijing,China [J].Science of the Total Environment,543(Pt A):326-335
Tian S L,Pan Y P,Wang Y S.2017.Size-resolved source apportionment of particulate matter in urban Beijing during haze and non-haze episodes[J].Atmospheric Chemistry & Physics Discussions,16(1):9405-9443
Wang Q,He X,Huang X H H,et al.Impact of secondary organic aerosol tracers on tracer-based source apportionment of organic carbon and PM2.5: A case study in the Pearl River Delta,China[J] ACS Earth Space Chemistry,1:562-571
Wang F,Lin T,Feng J,et al.2015.Source apportionment of polycyclic aromatic hydrocarbons in PM2.5 using positive matrix factorization modeling in Shanghai,China[J].Environmental Science Processes & Impacts,17(1):197-205
Wang Y,Li L,Chen C,et al.2014.Source apportionment of fine particulate matter during autumn haze episodes in Shanghai,China [J].Journal of Geophysical Research Atmospheres,119(4):1903-1914
王琴,张大伟,刘保献,等.2015.基于PMF模型的北京市PM2.5来源的时空分布特征[J].中国环境科学,35(10):2917-2924
Xie Y L,Hopke P K,Paatero P,et al.1999.Identification of source nature and seasonal variations of Arctic aerosol by the multilinear engine[J].Atmospheric Environment,33(16):2549-2562
Yao L,Yang L,Yuan Q,et al.2016.Sources apportionment of PM2.5,in a background site in the North China Plain[J].Science of the Total Environment,541:590-598
Yu J Z,Lau A K H,Louie K K,et al.2004.Abundance and seasonal characteristics of elemental and organic carbon in Hong Kong PM10[J].Atmospheric Environment,38(10):1511-1521
Yuan Z,Lau A K H,Zhang H,et al.2006.Identification and spatiotemporal variations of dominant PM10,sources over Hong Kong [J].Atmospheric Environment,40(10):1803-1815
Yuan Z,Yadav V,Turner J R,et al.2013.Long-term trends of ambient particulate matter emission source contributions and the accountability of control strategies in Hong Kong over 1998—2008[J].Atmospheric Environment,76(3):21-31
Zhang Y,Jing C,Wang S,et al.2017.Review of receptor-based source apportionment research of fine particulate matter and its challenges in China[J].Science of the Total Environment,586:917-929
Zhang R,Jing J,Tao J,et al.2013.Chemical characterization and source apportionment of PM2.5 in Beijing: seasonal perspective[J].Atmospheric Chemistry & Physics,13(14):7053-7074
Zíková N,Wang Y,Yang F,et al. 2016.On the source contribution to Beijing PM2.5 concentrations [J].Atmospheric Environment,134:84-95
郑君瑜,王水胜,黄志炯,等.2013.区域高分辨率大气排放源清单建立的技术方法与应用[M].北京:科学出版社
张延君,郑玫,蔡靖,等.2015.PM2.5源解析方法的比较与评述[J].科学通报,(2):109-121