红外掩日遥感监测炼油厂非甲烷烷烃排放通量

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摘要采用红外掩日通量遥感监测(SOF)技术分别在2014年5月~2015年12月和2021年10月监测了我国7座大型炼油厂(其中6座原油年加工量均超过1000万t)非甲烷烷烃排放通量(kg/h)及分布.每座炼油厂监测3~8d,测量18~73次,总计获得328个排放通量测量数据,根据国内炼油厂VOCs排放烟羽中非甲烷烷烃质量分数估算了VOCs排放量,结合监测期间实际原油加工量计算了非甲烷烷烃和VOCs排放系数.结果显示:7座炼油厂2014~2015年的非甲烷烷烃排放系数测定值为0.016%~0.11%,平均为0.081%;VOCs排放系数估算为0.020%~0.14%,平均为0.10%.无组织排放约占炼油厂非甲烷烷烃排放总量的70%以上,其中轻油贮罐排放占比过半.国内7座炼油厂2014~2015年非甲烷烷烃排放系数的最好水平与美国南加州6座炼油厂同期SOF监测的最好水平相当,但非甲烷烷烃排放系数的平均水平约为其平均水平的3.9倍,国内炼油厂的VOCs排放控制水平更加参差不齐.国内1座千万吨级炼油厂2021年监测的非甲烷烷烃排放通量和排放系数分别较2015年削减72.4%和74.2%.SOF可为石化VOCs无组织排放监测、量化和排放清单修订提供最佳实用技术,本研究结果提供了国内石化行业VOCs综合整治初期典型炼油厂非甲烷烷烃和VOCs的基线排放实测数据,以及1座千万t级炼油厂6a后治理攻坚效果.

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关键词 ：炼油厂, 非甲烷烷烃, VOCs, 无组织排放, 排放通量监测, 红外掩日通量遥感监测

Abstract：The emission fluxes (kg/h) and distributions of total non-methane alkanes from seven major refineries (in which six refineries were processing crude oil more than ten million tons per year) in China were quantified during May 2014 and December 2015 and in October 2021 using the Solar Occultation Flux (SOF) method. At each refinery site, 18~73measurement transects were performed during three to eight individual measurement days. In total, 328measurements of total non-methane alkane emission flux were performed for the seven refineries. Total VOC emissions were estimated from the measured total non-methane alkane emissions based on the average mass fraction of non-methane alkanes in total volatile organic compounds (VOC) measured in VOC emission plumes of several refineries in China. Total non-methane alkanes and VOC emission factors were calculated by scaling measured emissions of total non-methane alkanes and estimated emissions of VOCs with crude oil processing rates during the measurement period. The monitoring results indicate that the measured total non-methane alkanes emission factors ranged from 0.016% to 0.11% for the seven studied refineries and were 0.081% on average. The estimated VOC emission factors for the seven studied refineries ranged from 0.020% to 0.14%, with an average value of 0.10% during 2014 and 2015. Fugitive emissions accounted for more than 70% of total non-methane alkane emissions from refineries, and light oil tanks contributed more than 50% of fugitive non-methane alkane emissions. The results were compared to SOF measurements at six refineries in the South Coast Air Quality Management District (SCAQMD) in 2015, and the lowest level of total non-methane alkane emission factors in the seven refineries in China measured during 2014 and 2015 was the same as that for all six refineries in SCAQMD. However, the average level of total non-methane alkane emission factors of the seven refineries in China was 3.9times higher than that of the six refineries in SCAQMD, and there was a higher variability in total non-methane alkane emission factors among the seven refineries in China. The emission flux and emission factor of non-methane alkanes monitored in a major Chinese refinery in 2021 showed a reduction by 72.4% and 74.2% respectively compared with 2015. SOF could be developed as the best available technique for monitoring and quantifying fugitive and diffuse VOC emissions from petroleum and petrochemical industrial sites, and for revising VOC emission inventories. This study has provided a baseline of measured emissions of total non-methane alkanes and VOCs from typical refineries in the initial stage of VOC emissions control actions implemented in China in 2015, and VOCs control effectiveness of a major refinery after 6 years.

Key words： refinery non-methane alkanes volatile organic compounds diffuse and fugitive emission emission flux measurement solar occultation flux (SOF)

收稿日期: 2021-12-23

PACS:	X831
	X87

基金资助:中国石油化工股份有限公司科技开发项目(CLY15070,319006-6)

通讯作者: 李凌波,教授级高级工程师,lilingbo.fshy@sinopec.com E-mail: lilingbo.fshy@sinopec.com

作者简介: 李凌波(1969-),男,内蒙莫旗人,教授级高级工程师,工学学士,主要从事石油石化环境监测及污染物组学研究.发表论文40余篇.

引用本文:

李凌波, 宫超, 程梦婷, 李龙, 刘新宇. 红外掩日遥感监测炼油厂非甲烷烷烃排放通量[J]. 中国环境科学, 2022, 42(7): 3046-3057. LI Ling-bo, GONG Chao, CHENG Meng-ting, LI Long, LIU Xin-yu. Measurement of emission fluxes of total non-methane alkanes from refineries using solar occultation flux remote sensing technique. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(7): 3046-3057.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2022/V42/I7/3046

[1]	Li M, Zhang Q, Zheng B, et al. Persistent growth of anthropogenic non-methane volatile organic compound (NMVOC) emissions in China during 1990~2017:drivers, speciation and ozone formation potential[J]. Atmos Chem Phys, 2019,19:8897-8913.
[2]	环境保护部办公厅.环办
	[2015] 104号关于印发《石化行业VOCs污染源排查工作指南》及《石化企业泄漏检测与修复工作指南》的通知[EB/OL]. https://www.mee.gov.cn/gkml/hbb/bgt/201511/t20151124_317577.htm. 2015-11-17. Office of the Ministry of Environmental Protection. Huan Ban
	[2015] No. 104Notice on issuing《Guidelines for investigation of VOCs Pollution Sources in petrochemical industry》and《Guidelines for leak detection and repair in petrochemical enterprises》[EB/OL]. https://www.mee.gov.cn/gkml/hbb/bgt/201511/t20151124_317577.htm. 2015-11-17.
[3]	李凌波,程梦婷,李龙,等.炼油企业挥发性有机物无组织排放通量监测的现状与发展[J].中国环境监测, 2020,36(3):19-28. Li L, Cheng M, Li L, et al. Current and future developments in fugitive volatile organic compounds emission flux monitoring in petroleum refining industry[J]. Environmental Monitoring in China, 2020,36(3):19-28.
[4]	Simayi M, Hao Y, Li J, et al. Historical volatile organic compounds emission performance and reduction potentials in China's petroleum refining industry[J]. Journal of Cleaner Production, 2021,292:125810.
[5]	U.S.Environmental Protection Agency.AP-42:Compilation of Air Emissions Factors[EB/OL]. https://www.epa.gov/air-emissionsfactors-and-quantification/ap-42-compilation-air-emissions-factors.
[6]	Nelson T P. An examination of historical air pollutant emissions from US petroleum refineries[J]. Environmental Progress&Sustainable Energy, 2013,32(2):425-432.
[7]	Cuclis A. Why emission factors don't work at refineries and what to do about it[EB/OL]. https://www3.epa.gov/ttnchie1/conference/ei20/session7/acuclis.pdf. 2012.
[8]	Karl T, Striednig M, Graus M, et al. Urban flux measurements reveal a large pool of oxygenated volatile organic compound emissions[J]. Proc Natl Acad Sci USA, 2018,115(6):1186-1191.
[9]	环境保护部.公告2014年第55号关于发布《大气细颗粒物一次源排放清单编制技术指南(试行)》等4项技术指南的公告附件2大气挥发性有机物源排放清单编制技术指南(试行)[EB/OL]. https://www.mee.gov.cn/gkml/hbb/bgg/201408/t20140828_288364.htm. 2014-08-28. Ministry of Environmental Protection. Announcement
	[2014] No. 55 on Issuing four technical guidelines including《Technical guidelines for the preparation of emission inventories of atmospheric fine particulate matter from primary sources (trial implementation)》,Annex 2《Technical guidelines for the preparation of emission inventories of atmospheric volatile organic compounds (trial implementation)》[EB/OL]. https://www.mee.gov.cn/gkml/hbb/bgg/201408/t20140828_288364.htm. 2014-08-28.
[10]	U.S. Environmental Protection Agency Office of Air Quality Planning and Standards Air Quality Assessment Division Measurement Technology Group. EPA Handbook:Optical and remote sensing for measurement and monitoring of emissions flux of gases and particulate matter[EB/OL]. https://www.epa.gov/sites/production/files/2018-08/documents/gd-52v.2.pdf.
[11]	Robinson R, Gardiner T, Innocenti F, et al. Infrared differential absorption Lidar (DIAL) measurements of hydrocarbon emissions[J]. Journal of Environmental Monitoring, 2011,13:2213-2220.
[12]	Johansson J K E, Mellqvist J, Samuelsson J, et al. Emission measurements of alkenes, alkanes, SO2, and NO2 from stationary sources in Southeast Texas over a 5year period using SOF and mobile DOAS[J]. J Geophys Res Atmos, 2014,119:1973-1991.
[13]	Robinson R, Innocenti F, Helmore J, et al. The development and validation of a new standardized method for monitoring diffuse and fugitive VOC emissions from oil and gas facilities[C]. AWMA 2019 Air Quality Measurement Methods and Technology, April 2-4, 2019.Durham,NC.
[14]	European Committee for Standardization (CEN). EN 17628:2022 Fugitive and diffuse emissions of common concern to industry sectors-Standard method to determine diffuse emissions of volatile organic compounds into the atmosphere[S]. April 2022.
[15]	Wang F, Du W, Lv S, et al. Spatial and temporal distributions and sources of anthropogenic NMVOCs in the atmosphere of China:a review[J]. Advances in Atmosphere Science, 2021,38(7):1085-1100.
[16]	Wei W, Cheng S, Li G, et al. Characteristics of ozone and ozone precursors (VOCs and NOx) around a petroleum refinery in Beijing, China[J]. Journal of Environmental Sciences, 2014,26:332-342.
[17]	Lv D, Lu S, Tan X, et al. Source profiles, emission factors and associated contributions to secondary pollution of volatile organic compounds (VOCs) emitted from a local petroleum refinery in Shandong[J]. Environmental Pollution, 2021,274:116589.
[18]	Zhang Z, Wang H, Chen D, et al. Emission characteristics of volatile organic compounds and their secondary organic aerosol formation potentials from a petroleum refinery in Pearl River Delta, China[J]. Science of the Total Environment, 2017,584-585:1162-1174.
[19]	Lv D, Lu S, He S, et al. Research on accounting and detection of volatile organic compounds from a typical petroleum refinery in Hebei, North China[J]. Chemosphere, 2021,281:130653.
[20]	Zhang G, Wang N, Jiang X, et al. Characterization of ambient volatile organic compounds (VOCs) in the area adjacent to a petroleum refinery in Jinan, China[J]. Aerosol and Air Quality Research, 2017, 17:944-950.
[21]	李勤勤,张志娟,李杨,等.石油炼化无组织VOCs的排放特征及臭氧生成潜力分析[J].中国环境科学, 2016,36(5):1323-1331. Li Q, Zhang Z, Li Y, et al. Characteristics and ozone formation potential of fugitive volatile organic compounds (VOCs) emitted from petrochemical industry in Pearl River Delta[J]. China Environmental Science, 2016,36(5):1323-1331.
[22]	吕兆丰,魏巍,杨干,等.某石油炼制企业VOCs排放源强反演研究[J].中国环境科学, 2015,35(10):2958-2963. Lv Z, Wei W, Yang G, et al. Inversion research in VOCs source emission of a petroleum refinery[J]. China Environmental Science, 2015,35(10):2958-2963.
[23]	孙筱强,程水源,魏巍,等.炼油厂VOCs排放及其对O3生成的敏感性研究[J].安全与环境学报, 2011,11(6):101-105. Sun X, Cheng S, Wei W, et al. Research on the refinery O3 variation characteristics and VOCs reactivity[J]. Journal of Safety and Environment, 2011,11(6):101-105.
[24]	Pikelnaya O, Tsai C, Polidori A, et al. Understanding seasonal variations in refinery voc emissions using quarterly optical remote sensing mobile surveys[C]//AWMA 2019 Air Quality Measurement Methods and Technology. April 2-4, 2019.Durham,NC.
[25]	Mellqvist J, Samuelsson J, Isoz O, et al. Emission measurements of VOCs, NO2 and SO2 from the refineries in the south coast air basin using solar occultation flux and other optical remote sensing methods[EB/OL]. http://www.aqmd.gov/fenceline-monitoring/project-1.
[26]	李凌波,刘忠生,方向晨,等.炼油厂VOC排放控制策略-设备与管阀件泄漏[J].当代石油石化, 2013,21(9):1-9. Li L, Liu Z, Fang X, et al. Strategies of refinery VOC emission control-equipment leaks[J]. Petroleum&Petrochemical Today, 2013,21(9):1-9.
[27]	李凌波,刘忠生,方向晨.炼油厂VOC排放控制策略-储运、废水处理、工艺尾气、冷却塔及火炬[J].当代石油石化, 2013,(10):4-12. Li L, Liu Z, Fang X. The strategies for refinery VOC emission control-storage tanks and transfer operations, wastewater treatment, process vents, cooling towers and flares[J]. Petroleum&Petrochemical Today, 2013,21(10):4-12.
[28]	Barthe P, Chaugny M, Roudier S, et al. Best available techniques (BAT) reference document for the refining of mineral oil and gas. Industrial Emissions Directive 2010/75/EU (Integrated Pollution Prevention and control)[EB/OL]. 2015. http://eippcb.jrc.ec.europa.eu/reference/BREF/REF_BREF_2015.pdf.
[29]	Roveda L, Polvara E, Invernizzi M, et al. Definition of an emission factor for VOC emitted from Italian and European refineries[J]. Atmosphere, 2020,11(6):564-576.
[30]	Acton W J F, Huang Z, Davison B, et al. Surface-atmosphere fluxes of volatile organic compounds in Beijing[J]. Atmos. Chem. Phys., 2020,20:15101-15125.
[31]	Ryerson T B, Trainer M, Angevine W M, et al. Effect of petrochemical industrial emissions of reactive alkenes and NOx on tropospheric ozone formation in Houston, Texas[J]. J. Geophys. Res., 2003, 108(D8):4249.
[32]	Henry R C, Spiegelman C H, Collins J F, et al. Reported emissions of organic gases are not consistent with observations[J]. Proc Natl Acad Sci USA, 1997,94:6596-6599.
[33]	Li S M, Leithead A, Moussa S G, et al. Differences between measured and reported volatile organic compound emissions from oil sands facilities in Alberta, Canada[J]. Proc. Natl. Acad. Sci. USA, 2017,114(19):E3756-E3765.
[34]	Porter J, Tsai C, Pikelnaya O, et al. Routine direct measurements of refinery emissions of total alkanes over the last 5years in the Los Angeles air basin[C]//AGU Fall Meeting 2020.December 1-17, 2020.
[35]	Johansson J K E, Mellqvist J, Samuelsson J, et al. Quantitative measurements and modeling of industrial formaldehyde emissions in the Greater Houston area during campaigns in 2009 and 2011[J]. J. Geophys. Res. Atmos., 2014,119:4303-4322.
[36]	European Committee for Standardization (CEN).CEN/TC 264/WG 38"Determination of diffuse VOC emissions" Final Report[EB/OL]. https://www.vdi.de/fileadmin/pages/vdi_de/redakteure/ueber_uns/fachgesellschaften/KRdL/dateien/WG_38_Final_Report_SACEN2014-07.pdf.
[37]	Kille N. Development of solar occultation flux spectroscopy for ground and airborne applications[D]. Colorado:University of Colorado, 2020.
[38]	Mellqvist J, Samuelsson J, Johansson J, et al. Measurements of industrial emissions of alkenes in Texas using the solar occultation flux method[J]. J. Geophys. Res., 2010,115:D00F17.
[39]	Mellqvist J, Samuelsson J, Andersson P, et al. Using solar occultation flux and other optical remote sensing methods to measure VOC emissions from a variety of stationary sources in the South Coast Air Basin[EB/OL]. http://www.aqmd.gov/docs/default-source/fenceline_monitroing/project_2/fluxsense_project2_2015_final_report.pdf.
[40]	Mellqvist J, Samuelsson J, Offerle B, et al. VOC emissions monitoring in the Lost Hills Vicinity, San Joaquin Valley[EB/OL]. https://ww2.arb.ca.gov/sites/default/files/2021-03/FluxSenseInc_CARB_18ISD023_SJV_final_update_201027.pdf.
[41]	Bela M M, Kille N, McKeen S A, et al. Quantifying carbon monoxide emissions on the scale of large wildfires[J]. Geophysical Research Letters, 2022,49:e2021GL095831.
[42]	Kille N, Zarzana K J, Alvarez J R, et al. The CU airborne solar occultation flux instrument:performance evaluation during BB-FLUX[J]. ACS Earth Space Chem., 2022,6:582-596.
[43]	Johansson J, Mellqvist J, Li L, et al. Quantification of industrial VOC emissions in China using solar occultation flux (SOF)[EB/OL]. https://meetingorganizer.copernicus.org/EGU2017/EGU2017-19062.pdf.
[44]	Kille N, Baidar S, Handley P, et al. The CU mobile solar occultation flux instrument:structure functions and emission rates of NH3, NO2 and C2H6[J]. Atmos. Meas. Tech., 2017,10:373-392.
[45]	Degouw J A, Hekkert S T, Mellqvist J, et al. Airborne measurements of ethene from industrial sources using laser photo-acoustic spectroscopy[J]. Environ. Sci. Technol., 2009,43:2437-2442.