基于实地调研的广东省工业VOC排放清单改进研究
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摘要
工业源是人为源挥发性有机物(VOC)排放的重要贡献源,然而现有基于统计年鉴数据建立的工业VOC排放清单仍然存在排放源缺失、排放量低估、空间分配精度不足等问题.为了提高清单表征及空间分配的精细度,本文在2014年基于统计年鉴数据建立的广东省工业VOC排放清单的基础上,利用问卷调研方式获取了12000多家工业企业的详细活动水平数据,对工业VOC排放表征与空间分配进行改进,进而建立了基于实地调研和统计年鉴数据相结合的2014年广东省工业VOC排放改进清单.结果表明,改进后广东省工业VOC清单排放量由500927 t增至716470 t,珠三角地区行业VOC排放量增加30%左右,非珠三角地区增加90%左右,其中,炼油及石化行业VOC排放量变化最为明显.改进前清单借助人口密度等空间地理信息为空间分配依据,导致部分VOC排放分配到工业源较少的居民区或市中心;改进后的空间分配优先采用基于经纬度信息的点源分配方法,点源调研数据使得分配后的工业VOC主要集中在工业园区,少数工业VOC排放分配给人类活动有限的偏远农村地区,分配结果更为合理、精细.利用CAMx模型结合实际观测站点监测结果评估此次改进对O_3生成的影响,总体上改进后清单提高了广州、东莞、惠州和茂名等城市的O_3峰值期的模拟浓度,降低了东莞及广州O_3污染时期的模拟偏差,部分被低估的模拟峰值可以提高6～9μg·m~(-3);同时,空间分配的改进也影响了城市间O_3传输模拟.
Industrial source was one of the largest contributors to anthropogenic VOC emissions. However, the industrial VOC emission inventory, mainly developed based on the statistical yearbook, was typically underestimated and had high uncertainty in spatial allocation. This study proposed an emission update method that combines the statistical yearbook data and field investigation or survey data to refine the estimation and spatial allocation of the industrial VOC emission inventory. The method was used to refine the 2014-based industrial VOC emissions in Guangdong Province as a case study, in which more than 12000 detailed activity data of industries was used.Results show that the updated industrial VOC emissions increased from 500927 tons to 716470 tons, increased by 30% in the Pearl River Delta region and 90% in the Non Pearl River Delta region.Oil refining and petrochemical industry VOC emissions saw the most obvious change. Surrogate data, such as population density data, was typically used for spatial allocation of industrial VOC emissions. But it might inappropriately allocate the industrial VOC emissions into the downtown or residential areas where there are few VOC industrial emission sources. Using the update method, most industrial VOC emissions were allocated to the industry zone according to the detailed location information of industry. Only few of industrial VOC emissions were allocated to urban areas and remote areas with few human activities. Obviously, the spatial allocation of industrial VOC emissions using the update method is more reasonable. Finally, the impact of updated industrial VOC emissions on O_3 simulations were investigated using the CAMx model. Analysis was made from its results compared with monitoring data. It turns out that the updated industrial VOC emissions enhanced O_3 simulation during peak periods particularly in Guangzhou, Dongguan, Huizhou and Maoming City, and reduced the simulation error of the peak period when ozone pollution occurs in Guangzhou and Dongguan. Underestimated O_3 simulation could be increased by 6～9 μg·m~(-3) during the pollution peak period. Meanwhile, the optimization of spatial allocation could influence regional transport of O_3.
Industrial source was one of the largest contributors to anthropogenic VOC emissions. However, the industrial VOC emission inventory, mainly developed based on the statistical yearbook, was typically underestimated and had high uncertainty in spatial allocation. This study proposed an emission update method that combines the statistical yearbook data and field investigation or survey data to refine the estimation and spatial allocation of the industrial VOC emission inventory. The method was used to refine the 2014-based industrial VOC emissions in Guangdong Province as a case study, in which more than 12000 detailed activity data of industries was used.Results show that the updated industrial VOC emissions increased from 500927 tons to 716470 tons, increased by 30% in the Pearl River Delta region and 90% in the Non Pearl River Delta region.Oil refining and petrochemical industry VOC emissions saw the most obvious change. Surrogate data, such as population density data, was typically used for spatial allocation of industrial VOC emissions. But it might inappropriately allocate the industrial VOC emissions into the downtown or residential areas where there are few VOC industrial emission sources. Using the update method, most industrial VOC emissions were allocated to the industry zone according to the detailed location information of industry. Only few of industrial VOC emissions were allocated to urban areas and remote areas with few human activities. Obviously, the spatial allocation of industrial VOC emissions using the update method is more reasonable. Finally, the impact of updated industrial VOC emissions on O_3 simulations were investigated using the CAMx model. Analysis was made from its results compared with monitoring data. It turns out that the updated industrial VOC emissions enhanced O_3 simulation during peak periods particularly in Guangzhou, Dongguan, Huizhou and Maoming City, and reduced the simulation error of the peak period when ozone pollution occurs in Guangzhou and Dongguan. Underestimated O_3 simulation could be increased by 6～9 μg·m~(-3) during the pollution peak period. Meanwhile, the optimization of spatial allocation could influence regional transport of O_3.
引文
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Duan J,Tan J,Yang L,et al.2008.Concentration,sources and ozone formation potential of volatile organic compounds (VOCs) during ozone episode in Beijing[J].Atmospheric Research,88(1):25-35
Fu X,Wang S,Zhao B,et al.2013.Emission inventory of primary pollutants and chemical speciation in 2010 for the Yangtze River Delta region,China[J].Atmospheric Environment,70(70):39-50
Huang C,Chen C H,Li L,et al.2011.Emission inventory of anthropogenic air pollutants and VOC species in the Yangtze River Delta region,China[J].Atmospheric Chemistry and Physics,11(9):4105-4120
Li J,Lu K,Lv W,et al.2014.Fast increasing of surface ozone concentrations in Pearl River Delta characterized by a regional air quality monitoring network during 2006—2011[J].Journal of Environmental and Science (China),26(1):23-36
李璇,王雪松,刘中,等.2014.宁波人为源VOC清单及重点工业行业贡献分析[J].环境科学,35(7):2497-2502
刘金凤,赵静,李湉湉,等.2008.我国人为源挥发性有机物排放清单的建立[J].中国环境科学,28(6):496-500
Ou J,Zheng J,Li R,et al.2015.Speciated OVOC and VOC emission inventories and their implications for reactivity-based ozone control strategy in the Pearl River Delta region,China[J].Science of the Total Environment,530-531:393-402
潘月云,李楠,郑君瑜,等.2015.广东省人为源大气污染物排放清单及特征研究[J].环境科学学报,35(9):2655-2669
Pouliot G,Wisner E,Mobley D,et al.2012.Quantification of emission factor uncertainty.[J].Journal of the Air & Waste Management Association,62(3):287-298
钱伟,蔡慧华,余宇帆,等.2015.广东省石化行业挥发性有机化合物排放污染及治理现状[J].广东化工,42(8):37-39
沈劲,黄晓波,汪宇,等.2017.广东省臭氧污染特征及其来源解析研究[J].环境科学学报,37(12):4449-4457
王红丽.2015.上海市大气挥发性有机物化学消耗与臭氧生成的关系[J].环境科学,36(9):3159-3167
魏巍,王书肖,郝吉明.2011.中国人为源VOC排放清单不确定性研究[J].环境科学,32(2):305-312
Wu R,Bo Y,Li J,et al.2016.Method to establish the emission inventory of anthropogenic volatile organic compounds in China and its application in the period 2008—2012[J].Atmospheric Environment,127:244-254
叶绿萌,樊少芬,常鸣,等.2016.珠三角地区秋季臭氧生成敏感性时空变化模拟研究[J].南京大学学报(自然科学),52(6):977-988
余宇帆,卢清,郑君瑜,等.2011.珠江三角洲地区重点VOC排放行业的排放清单[J].中国环境科学,31(2):195-201
Yin S,Zheng J,Lu Q,et al.2015.A refined 2010-based VOC emission inventory and its improvement on modeling regional ozone in the Pearl River Delta Region,China[J].Science of the Total Environment,514:426-438
Zheng J,Shao M,Che W,et al.2009.Speciated VOC Emission Inventory and Spatial Patterns of Ozone Formation Potential in the Pearl River Delta,China[J].Environmental Science & Technology,43(22):8580-8586
Zhong Z,Zheng J,Zhu M,et al.2018.Recent developments of anthropogenic air pollutant emission inventories in Guangdong province,China[J].Science of the Total Environment,627:1080-1092
钟流举,郑君瑜,雷国强,等.2007.大气污染物排放源清单不确定性定量分析方法及案例研究[J].环境科学研究,20(4):15-20
Duan J,Tan J,Yang L,et al.2008.Concentration,sources and ozone formation potential of volatile organic compounds (VOCs) during ozone episode in Beijing[J].Atmospheric Research,88(1):25-35
Fu X,Wang S,Zhao B,et al.2013.Emission inventory of primary pollutants and chemical speciation in 2010 for the Yangtze River Delta region,China[J].Atmospheric Environment,70(70):39-50
Huang C,Chen C H,Li L,et al.2011.Emission inventory of anthropogenic air pollutants and VOC species in the Yangtze River Delta region,China[J].Atmospheric Chemistry and Physics,11(9):4105-4120
Li J,Lu K,Lv W,et al.2014.Fast increasing of surface ozone concentrations in Pearl River Delta characterized by a regional air quality monitoring network during 2006—2011[J].Journal of Environmental and Science (China),26(1):23-36
李璇,王雪松,刘中,等.2014.宁波人为源VOC清单及重点工业行业贡献分析[J].环境科学,35(7):2497-2502
刘金凤,赵静,李湉湉,等.2008.我国人为源挥发性有机物排放清单的建立[J].中国环境科学,28(6):496-500
Ou J,Zheng J,Li R,et al.2015.Speciated OVOC and VOC emission inventories and their implications for reactivity-based ozone control strategy in the Pearl River Delta region,China[J].Science of the Total Environment,530-531:393-402
潘月云,李楠,郑君瑜,等.2015.广东省人为源大气污染物排放清单及特征研究[J].环境科学学报,35(9):2655-2669
Pouliot G,Wisner E,Mobley D,et al.2012.Quantification of emission factor uncertainty.[J].Journal of the Air & Waste Management Association,62(3):287-298
钱伟,蔡慧华,余宇帆,等.2015.广东省石化行业挥发性有机化合物排放污染及治理现状[J].广东化工,42(8):37-39
沈劲,黄晓波,汪宇,等.2017.广东省臭氧污染特征及其来源解析研究[J].环境科学学报,37(12):4449-4457
王红丽.2015.上海市大气挥发性有机物化学消耗与臭氧生成的关系[J].环境科学,36(9):3159-3167
魏巍,王书肖,郝吉明.2011.中国人为源VOC排放清单不确定性研究[J].环境科学,32(2):305-312
Wu R,Bo Y,Li J,et al.2016.Method to establish the emission inventory of anthropogenic volatile organic compounds in China and its application in the period 2008—2012[J].Atmospheric Environment,127:244-254
叶绿萌,樊少芬,常鸣,等.2016.珠三角地区秋季臭氧生成敏感性时空变化模拟研究[J].南京大学学报(自然科学),52(6):977-988
余宇帆,卢清,郑君瑜,等.2011.珠江三角洲地区重点VOC排放行业的排放清单[J].中国环境科学,31(2):195-201
Yin S,Zheng J,Lu Q,et al.2015.A refined 2010-based VOC emission inventory and its improvement on modeling regional ozone in the Pearl River Delta Region,China[J].Science of the Total Environment,514:426-438
Zheng J,Shao M,Che W,et al.2009.Speciated VOC Emission Inventory and Spatial Patterns of Ozone Formation Potential in the Pearl River Delta,China[J].Environmental Science & Technology,43(22):8580-8586
Zhong Z,Zheng J,Zhu M,et al.2018.Recent developments of anthropogenic air pollutant emission inventories in Guangdong province,China[J].Science of the Total Environment,627:1080-1092
钟流举,郑君瑜,雷国强,等.2007.大气污染物排放源清单不确定性定量分析方法及案例研究[J].环境科学研究,20(4):15-20