专题论文

上海大气中气相和颗粒相羰基化合物研究

  • 王芳 ,
  • 冯艳丽 ,
  • 姜知明 ,
  • 仇奕沁 ,
  • 陈颖军
展开
  • 1. 上海大学环境与化学工程学院, 上海200444;
    2. 中国科学院烟台海岸带研究所, 烟台264003
王芳,硕士研究生,研究方向为大气羰基化合物,电子信箱wangfang.shu@qq.com

收稿日期: 2015-02-09

  修回日期: 2015-02-26

  网络出版日期: 2015-04-10

基金资助

国家自然科学基金项目(41173098, 41273135)

Gaseous and particulate carbonyl compounds in Shanghai ambient air

  • WANG Fang ,
  • FENG Yanli ,
  • JIANG Zhiming ,
  • QIU Yiqin ,
  • CHEN Yingjun
Expand
  • 1. School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, China;
    2. Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai 264003, China

Received date: 2015-02-09

  Revised date: 2015-02-26

  Online published: 2015-04-10

摘要

为探究大气中羰基化合物的质量浓度水平及变化规律, 利用滤膜系统(FP)同时采集大气中颗粒相和气相羰基化合物, FP系统由3 层47 mm 滤膜组成, 其中, 第1 层滤膜用于收集颗粒相羰基化合物, 第2 层和第3 层滤膜涂布五氟苄基羟胺(PFBHA)衍生剂, 用于收集气相羰基化合物。PFBHA 的涂布量为12 μmol、采样流速4 L/min, 每个样品采集4 h。采集后的样品用正己烷提取。利用该方法对上海市大气中的羰基化合物进行研究, 结合气相色谱/质谱仪(GC/MS), 分析大气中羰基化合物浓度的日变化、季节变化以及气相-颗粒相分配规律。研究结果表明:1)上海市大气中15 种目标化合物均能检测到, 包括13 种单羰基化合物和2 种二羰基化合物;2)上海大气中羰基化合物具有明显的日变化和季节变化, 气相羰基化合物的浓度在中午达到最大值, 颗粒相则相反;夏季羰基化合物的总质量浓度((33.8±15.9)μg/m3)显著高于冬季和春季(分别为(10.5±5.0)和(14.0±7.0)μg/m3);3)羰基化合物的气粒分配规律表现为与温度呈正相关、与相对湿度呈负相关。本研究表明, FP 系统可替代AD-FP(环形溶蚀器-滤膜系统)同时采集大气中气相和颗粒相中的羰基化合物, 易于携带, 为羰基化合物的野外观测提供便利。

本文引用格式

王芳 , 冯艳丽 , 姜知明 , 仇奕沁 , 陈颖军 . 上海大气中气相和颗粒相羰基化合物研究[J]. 科技导报, 2015 , 33(6) : 13 -19 . DOI: 10.3981/j.issn.1000-7857.2015.06.001

Abstract

In order to explore the concentration levels and variations of carbonyl compounds in the atmosphere, a filter pack (FP) system was used to collect gaseous and particulate carbonyl compounds simultaneously in Shanghai ambient air. There are three 47 mm filters in the FP system. Particulate carbonyls were collected on the first filter directly and then the gaseous carbonyls were collected on the second and third filters impregnated with PFBHA. The coating amount of PFBHA was 12 μmol, the sampling flow was 4 L·min-1 for 4 hours. The filter samples were extracted by hexane and injected into the GC/MS system. Seasonal and diurnal variations of carbonyl compounds as well as the gas-particle partitioning were studied. The results showed as follows: 1) 15 target carbonyl compounds are all detected in Shanghai ambient air, including 13 mono-carbonyls and 2 dicarbonyls; 2) the carbonyl compounds exhibit significant seasonal and diurnal variations with higher concentrations in summer, the concentrations of gaseous carbonyls reach the maximum at noon while the particle phases achieve the minimum values at the same time; the total concentration of carbonyls is 33.8±15.9 μg/m3 in summer, significantly higher than the levels in winter (10.5±5.0 μg/m3) and spring (14.0±7.0 μg/m3); 3) gas-particle partitioning of carbonyl compounds is found to be positively correlated with ambient temperature while negatively with relative humidity. Compared to the annular denuder-filter pack (AD-FP) system, the FP system is more suitable for field observation.

参考文献

[1] Shah J J, Johnson M C, Charlson R J, et al. Carbonaceous aerosol at urban and rural sites in the United States[J]. Air Pollution Control Association, 1986, 36(3): 254-257.
[2] Turpin B J, Saxena P, Andrews E. Measuring and simulating particulate organics in the atmosphere: Problems and prospects[J]. Atmospheric Environment, 2000, 34(18): 2983-3013.
[3] Penner J E, Dickenson R E, O'Neill C A. Effects of aerosol from biomass burning on the global radiation budget[J]. Science, 1992, 256(5062): 1432-1434.
[4] 汪午, 王省良, 李黎, 等. 天然源二次有机气溶胶的研究进展[J]. 地球化 学, 2008, 37(1): 77-86. Wang Wu, Wang Shengliang, Li Li, et al. Advances in biogenic secondary organic aerosols[J]. Geochemical, 2008, 37(1): 77-86.
[5] Jang M, Czoschke N M, Lee S, et al. Heterogeneous atmospheric aerosol production by acid-catalyzed particle-phase reactions[J]. Science, 2002, 298(5594): 814-817.
[6] 邹婷, 冯艳丽, 付正茹, 等. 五氟苄基羟胺衍生与GC/MS联用分析大气 中的单羰基化合物和多羰基化合物[J]. 环境科学学报, 2012, 32(11): 2718-2724. Zou Ting, Feng Yanli, Fu Zhengru, et al. Determination of mono-and dicarbonyls in the atmosphere using gas chromatography/mass spectrometry after PFBHA derivatization[J]. Journal of Environmental Science, 2012, 32(11): 2718-2724.
[7] 冯艳丽, 牟翠翠, 付正茹, 等. 涂布2, 4-二硝基苯肼的环形溶蚀器/滤 膜系统和高效液相色谱法检测大气中二羰基化合物[J]. 分析化学, 2011, 39(11): 1653-1658. Feng Yanli, Mu Cuicui, Fu Zhengru, et al. Determination of airborne dicarbonyls by annular denuder/filter pack system coated with 2, 4-dinitrophenylhydrazine and high performance liquid chromatography[J]. Chinese Journal of Analytical Chemistry, 2011, 39(11): 1653-1658.
[8] 付正茹, 冯艳丽, 任青青, 等. 上海市大气PM2.5中羰基化合物的研究[J]. 中国环境科学, 2013, 33(11): 1937-1945. Fu Zhengru, Feng Yanli, Ren Qingqing, et al. Study of carbonyl compounds in the atmosphere of Shanghai[J]. China Environmental Science, 2013, 33(11): 1937-1945.
[9] Ho S S H, Ho K F, Liu W D, et al. Unsuitability of using the DNPHcoated solid sorbent cartridge for determination of airborne unsaturated carbonyls[J]. Atmospheric Environment, 2011, 45(1): 261-265.
[10] Feng Y L, Wen S, Chen T, et al. Ambient levels of carbonyl compounds and their sources in Guangzhou, China[J]. Atmospheric Environment, 2005, 39(10): 1789-1800.
[11] Pang X, Mu Y. Seasonal and diurnal variations of carbonyl compounds in Beijing ambient air[J]. Atmospheric Environment, 2006, 40(33): 6313-6320.
[12] Lü H X, Cai Q Y, Wen S, et al. Seasonal and diurnal variations of carbonyl compounds in the urban atmosphere of Guangzhou, China[J]. The Science of the Total Environment, 2010, 408(17): 3523-3529.
[13] Wang H K, Huang C H, Chen K S, et al. Measurement and source characteristics of carbonyl compounds in the atmosphere in Kaohsiung city, Taiwan[J]. Journal of Hazardous Materials, 2010, 179(1): 1115-1121.
[14] Weng M, Zhu L, Yang K, et al. Levels and health risks of carbonyl compounds in selected public places in Hangzhou, China[J]. Journal of Hazardous Materials, 2009, 164(2-3): 700-706.
[15] Temime B, Healy R M, Wenger J C, et al. A denuder-filter sampling technique for the detection of gas and particle phase carbonyl compounds[J]. Environmental Science Technology, 2007, 41(18): 6514-6520.
[16] Ortiz R, Shimada S, Sekiguchi K, et al. Measurements of changes in the atmospheric partitioning of bifunctional carbonyls near a road in a suburban area[J]. Atmospheric Environment, 2013, 81: 554-560.
[17] Kawamura K, Okuzawa K, Aggarwal S G, et al. Determination of gaseous and particulate carbonyls (glycolaldehyde, hydroxyacetone, glyoxal, methylglyoxal, nonanal and decanal) in the atmosphere at Mt. Tai[J]. Atmospheric Chemistry and Physics, 2013, 13(10): 5369-5380.
[18] Shee Y, Hee S S. Optimization of a solid sorbent dynamic personal air sampling method for aldehydes[J]. Applied Occupational and Environmental Hygiene, 2000, 15(2): 228-234.
[19] Ho S H H, Yu J Z. Determination of airborne carbonyls: Comparison of a thermal desorption/GC method with the standard DNPH/HPLC method[J]. Environmental Science Technology, 2004, 38(3): 862-870.
[20] 许嘉钰, 高阳. 北京市城区大气羰基化合物的季节变化[J]. 环境科学, 2009, 30(3): 625-630. Xu Jiayu, Gao Yang. Seasonal variations of carbonyl compounds in urban atmosphere of Beijing[J]. Environmental Science, 2009, 30(3): 625-630.
[21] Possanzini M, Di Palo V, Petricca R, et al. Measurements of lower carbonyls in Rome ambient air[J]. Atmospheric Environment, 1996, 30 (22): 3757-3764.
[22] Pang X B, Mu Y J, Yuan J. Carbonyls emission from ethanol-blended gasoline and biodiesel-ethanol-diesel used in engines[J]. Atmospheric Environment, 2008, 42(6): 1349-1358.
[23] Hu S, Yu J Z. Feasibility of collection and analysis of airborne carbonyls by on-sorbent derivatization and thermal desorption[J]. Analytical Chemistry, 2002, 74(6): 1232-1240.
[24] 任青青, 冯艳丽, 王芳, 等. 利用涂布五氟苄基羟胺(PFBHA)/XAD-4 的环形溶蚀器/滤膜系统和GC-MS分析大气中单羰基和二羰基化合 物[J]. 上海大学学报, 已接收. Ren Qingqing, Feng Yanli, Wang Fang, et al. Determination of monocarbonyl and dicarbonyl compounds in Shanghai atmosphere by annular denuder/filter pack system coated with XAD-4 and PFBHA using GC/MS[J]. Journal of Shanghai University, Accepted for Publication.
[25] Jang M, Kamens R M. Atmospheric secondary aerosol formation by heterogeneous reactions of aldehydes in the presence of a sulfuric acid aerosol catalyst[J]. Environmental Science Technology, 2001, 35(24): 4758-4766.
[26] Matsunaga S, Mochida M, Kawamura K. Variation on the atmospheric concentrations of biogenic carbonyl compounds and their removal processes in the northern forest at Moshiri, Hokkaido Island in Japan[J]. Journal of Geophysical Research-Atmosphere, 2004, 109(D4): 1-9.
[27] Bao L, Matsumoto M, Kubota T, et al. Gas/particle partitioning of lowmolecular-weight dicarboxylic acids at a suburban site in Saitama, Japan[J]. Atmospheric Environment, 2012, 47: 546-553.
文章导航

/