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浙江大学学报(工学版)
Journal of ZheJiang University (Engineering Science)  2019, Vol. 53 Issue (4): 671-683    DOI: 10.3785/j.issn.1008-973X.2019.04.008
    
Ambient VOCs characteristics and associated effects in urban Hangzhou
Kang-wei LI1(),Fang YING2,Ling-hong CHEN1,*(),Xian-jue ZHENG2,Li-xia HAN1,Xue-cheng WU1,Xiang GAO1,Ke-fa CEN1
1. State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, China
2. Hangzhou Environmental Monitoring Center Station, Hangzhou 310007, China
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Abstract  

Measurements of 56 volatile organic compounds (VOCs) species were obtained using online GC-FID/PID through one-year observation in urban Hangzhou in 2013. The VOCs composition, seasonal variation and diurnal cycles were analyzed. The annually averaged total VOCs was 42.1×10?9, with alkane accounting for 54%, followed by alkene (23.4%), aromatic (14.4%) and acetylene (8.2%). The diurnal cycles of VOCs showed lower values in daytime than nighttime, with minimum value at 14:00. Further analysis on typical species showed that the vehicle emissions were possibly regarded as the major VOCs source in urban Hangzhou. Both propene-equivalent concentration and ozone formation potential (OFP) analysis indicated that alkenes contributed over 60% of total VOCs reactivity. Associated meteorological effects showed that VOCs volume fractions were negative to temperature in 11-40 °C, while positive to relative humidity. Solar radiation has significant impact on VOCs values, while wet removal effect was not obvious. Eastern and northern winds were dominated for the whole year, but the volume fraction distribution of VOCs in different wind directions was not obvious. The VOCs volume fractions decreased as wind speed increased, regardless any wind direction. For different seasons, the impact extent of wind speed followed order as autumn>winter>spring>summer.

Key words： volatile organic compounds (VOCs)      urban pollution      diurnal cycle      ozone formation potential      meteorological effect     
Received: 28 December 2017      Published: 28 March 2019
CLC:  X 511  
Corresponding Authors: Ling-hong CHEN     E-mail: likangweizju@qq.com;chenlh@zju.edu.cn
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Kang-wei LI
Fang YING
Ling-hong CHEN
Xian-jue ZHENG
Li-xia HAN
Xue-cheng WU
Xiang GAO
Ke-fa CEN
Cite this article:

Kang-wei LI,Fang YING,Ling-hong CHEN,Xian-jue ZHENG,Li-xia HAN,Xue-cheng WU,Xiang GAO,Ke-fa CEN. Ambient VOCs characteristics and associated effects in urban Hangzhou. Journal of ZheJiang University (Engineering Science), 2019, 53(4): 671-683.

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http://www.zjujournals.com/eng/10.3785/j.issn.1008-973X.2019.04.008     OR     http://www.zjujournals.com/eng/Y2019/V53/I4/671


杭州市主城区VOCs污染特征及影响因素

采用在线气相色谱仪，2013年在杭州市主城区对56种挥发性有机物（VOCs）开展1年的连续观测. 研究VOCs组成、季节变化特征和日变化规律，总VOCs年均体积分数为42.1×10?9，其中烷烃占54.0%，烯烃占23.4%，芳香烃占14.4%，炔烃占8.2%. 日变化规律表现为夜晚体积分数高于白天，在14:00达到全天最低值. 分析VOCs特征物种发现，机动车尾气可能是主城区VOCs的主要来源. 丙烯等效体积分数和臭氧生成潜势（OFP）均表明，VOCs反应活性较大的是烯烃，对OH活性和OFP的贡献率均超过60%，其次芳香烃和烷烃. 分析气象要素与VOCs体积分数关系发现，在11~40 °C下VOCs体积分数随着温度的升高而降低，与湿度有明显的正相关. 光照对VOCs体积分数的影响较大，降水对VOCs的冲刷不明显. 杭州全年以东风、北风为主导风向，但不同风向下的VOCs体积分数分布规律不明显. 不论是主导还是非主导风向，VOCs体积分数始终随着风速的增大而减小，对于不同季节，风速影响幅度依次是秋季>冬季>春季>夏季.


关键词： 挥发性有机物,  城市污染,  日变化,  臭氧生成潜势,  气象要素 
Fig.1 Monthly averaged VOCs in urban Hangzhou
城市 时间 站点属性 ${\varphi _{\rm B}}$/% 文献
烷烃 烯烃 芳香烃 炔烃
注：表格中已剔除武汉和北京2个城市含氧VOCs和卤代烃的原始数据，并重新计算.
杭州 2013全年 城区 54.0 23.4 14.4 8.2 本文
北京 2014全年 城区 57.5 18.6 12.9 11.0 文献[20]
上海 2010全年 城区 46.7 11.3 33.2 8.8 文献[7]
南京 2013.3~2014.2 郊区 46.1 21.9 22.0 10.0 文献[8]
广州 2011.6~2012.5 城区 58.0 16.0 26.0 ? 文献[13]
武汉 2014.10 城区 54.8 20.8 13.7 10.7 文献[21]
Tab.1 Summary of ambient VOCs composition in typical cities in China
Fig.2 Seasonal and annual diurnal cycles of O3, NOx, VOCs, CO and typical VOC species
类别 物种 含碳数 kOH/1012 MIR VMR/10?9 Prop-Equiv/10?9 OFP/10?9
烷烃 乙烷 2 0.24 0.25 2.76 0.05 0.69
丙烷 3 1.10 0.48 4.59 0.58 2.20
异丁烷 4 2.34 1.21 4.17 1.48 5.05
正丁烷 4 2.54 1.02 3.20 1.23 3.26
异戊烷 5 3.90 1.38 1.68 1.24 2.32
正戊烷 5 3.94 1.04 1.01 0.76 1.05
环戊烷 5 5.16 2.40 0.81 0.79 1.94
2,2-二甲基丁烷 6 2.32 0.82 0.24 0.13 0.20
2,3-二甲基丁烷 6 6.30 1.07 3.32 4.78 3.56
2-甲基戊烷 6 5.60 1.50 0.69 0.88 1.04
3-甲基戊烷 6 5.70 1.50 0.86 1.12 1.29
正己烷 6 5.61 0.98 1.00 1.29 0.98
甲基环戊烷 6 7.05 2.80 2.29 3.68 6.40
环己烷 6 7.49 1.28 0.62 1.06 0.79
2,4-二甲基戊烷 7 5.10 1.50 1.96 2.67 2.95
正庚烷 7 7.15 0.81 0.75 1.43 0.61
甲基环己烷 7 10.4 1.80 0.40 1.10 0.72
2-甲基己烷 7 7.18 1.08 0.41 0.79 0.45
2,3-二甲基戊烷 7 1.31 0.21 0.69 0.24 0.15
3-甲基己烷 7 7.18 1.40 0.83 1.59 1.16
2,2,4-三甲基戊烷 8 3.68 0.93 0.33 0.37 0.31
2,3,4-三甲基戊烷 8 7.00 1.60 0.82 1.74 1.31
2-甲基庚烷 8 0.96 0.01 1.17 0.34 0.01
3-甲基庚烷 8 8.54 0.99 0.32 0.82 0.31
正辛烷 8 8.68 0.60 0.40 1.05 0.24
正壬烷 9 10.20 0.54 0.21 0.73 0.11
正葵烷 10 11.60 0.46 0.48 2.13 0.22
十一烷 11 13.20 0.42 0.33 1.85 0.14
烯烃 乙烯 2 8.52 9.00 4.95 3.21 44.54
丙烯 3 26.3 9.40 1.41 4.22 13.23
1-丁烯 4 31.4 8.90 0.73 3.48 6.48
烯烃 异丁烯 4 51.4 6.29 1.78 13.93 11.20
1,3-丁二烯 4 66.6 10.9 0.94 9.48 10.20
顺-2-丁烯 4 56.4 10 0.56 4.83 5.63
反-2-丁烯 4 64 10 0.64 6.22 6.39
1-戊烯 5 31.4 6.2 0.48 2.87 2.98
异戊二烯 5 101 9.1 3.72 71.48 33.88
顺-2-戊烯 5 65 8.8 0.23 2.82 2.01
反-2-戊烯 5 67 8.8 0.21 2.68 1.85
1-己烯 6 37 5.49 0.16 1.31 0.85
芳香烃 苯 6 1.23 0.42 0.91 0.25 0.38
甲苯 7 5.96 2.7 1.98 3.15 5.36
乙苯 8 7.1 2.7 1.56 3.37 4.21
对/间二甲苯 8 23.6 8.2 0.42 2.99 3.41
邻二甲苯 8 13.7 6.5 0.47 1.97 3.07
苯乙烯 8 10 2.2 0.62 1.89 1.37
异丙苯 9 6.5 2.2 0.23 0.50 0.50
正丙苯 9 6 2.1 0.23 0.46 0.47
1,3,5-三甲基苯 9 57.5 10.1 0.61 12.04 6.18
1,2,4-三甲基苯 9 32.5 8.8 0.31 3.42 2.71
间乙基甲苯 9 19.2 1.57 0.53 3.47 0.83
对乙基甲苯 9 12.1 1.15 0.79 3.28 0.91
邻乙基甲苯 9 12.3 0.14 0.37 1.56 0.05
1,2,3-三甲苯 9 32.7 8.9 0.45 5.06 4.03
间/对二乙苯 10 24.3 0.08 0.23 2.11 0.02
炔烃 乙炔 2 0.83 0.5 5.51 0.35 2.75
Tab.2 Annually averaged volume mixing ratio (VMR), propene-equivalent concentration (Prop-Equiv) and ozone formation potential (OFP) of 56 VOCs species
Fig.3 Seasonal and annual contribution of VOCs category to volume mixing ratio, propene-equivalent concentration and ozone formation potential
排序 化合物 VMR/10?9 P/% 化合物 Prop-Equiv/10?9 P/% 化合物 OFP/10?9 P/%
1 乙炔 5.5 8.2 异戊二烯 71.5 34.3 乙烯 44.5 20.7
2 乙烯 4.9 7.3 异丁烯 13.9 6.7 异戊二烯 33.9 15.8
3 丙烷 4.6 6.8 1,3,5-三甲基苯 12.0 5.8 丙烯 13.2 6.2
4 异丁烷 4.2 6.2 1,3-丁二烯 9.5 4.6 异丁烯 11.2 5.2
5 异戊二烯 3.7 5.5 反-2-丁烯 6.2 3.0 1,3-丁二烯 10.2 4.8
6 2,3-二甲基丁烷 3.3 4.9 1,2,3-三甲苯 5.1 2.4 1-丁烯 6.5 3.0
7 正丁烷 3.2 4.7 顺-2-丁烯 4.8 2.3 甲基环戊烷 6.4 3.0
8 乙烷 2.8 4.1 2,3-二甲基丁烷 4.8 2.3 反-2-丁烯 6.4 3.0
9 甲基环戊烷 2.3 3.4 丙烯 4.2 2.0 1,3,5-三甲基苯 6.2 2.9
10 甲苯 2.0 2.9 甲基环戊烷 3.7 1.8 顺-2-丁烯 5.6 2.6
11 2,4-二甲基戊烷 2.0 2.9 1-丁烯 3.5 1.7 甲苯 5.4 2.5
12 异丁烯 1.8 2.6 间乙基甲苯 3.5 1.7 异丁烷 5.0 2.4
13 异戊烷 1.7 2.5 1,2,4-三甲基苯 3.4 1.6 乙苯 4.2 2.0
14 乙苯 1.6 2.3 乙苯 3.4 1.6 1,2,3-三甲苯 4.0 1.9
15 丙烯 1.4 2.1 对乙基甲苯 3.3 1.6 2,3-二甲基丁烷 3.6 1.7
16 2-甲基庚烷 1.2 1.7 乙烯 3.2 1.5 对/间二甲苯 3.4 1.6
17 正戊烷 1.0 1.5 甲苯 3.1 1.5 正丁烷 3.3 1.5
18 正己烷 1.0 1.5 对/间二甲苯 3.0 1.4 邻二甲苯 3.1 1.4
19 1,3-丁二烯 0.9 1.4 1-戊烯 2.9 1.4 1-戊烯 3.0 1.4
20 苯 0.9 1.3 顺-2-戊烯 2.8 1.4 2,4-二甲基戊烷 2.9 1.4
Tab.3 Annual top 20 VOCs species based on volume mixing ratio, propene-equivalent concentration and ozone formation potential
Fig.4 Changes of VOCs volume fraction on temperature
Fig.5 Changes of VOCs volume fraction on relative humidity
Fig.6 Interaction of temperature, relative humidity and VOCs volume fraction
Fig.7 Interaction of daily average of VOCs volume fraction, daily maximum of solar radiation and daily maximum of O3 volume fraction
月份 降水天数/d 降水量/mm ${\varphi _{\rm t }}$（VOCs）/10?9 相对变化/% ${\varphi _{\rm s}} $（VOCs）/10?9 相对变化/%
非降水期间 降水期间 非降水期间 降水期间
1 6 24.9 45.6 80.9 77.2 37.9 64.8 71.0
2 17 66.8 29.3 30.5 4.0 23.6 26.3 11.4
3 13 115.9 43.1 43.0 ?0.1 28.0 38.2 36.3
4 8 98.1 37.7 33.2 ?11.9 28.1 33.3 18.3
5 10 121.3 39.2 34.8 ?11.3 27.5 33.8 22.9
6 18 346 38.1 41.0 7.5 31.6 37.7 19.3
7 3 9.3 37.6 32.3 ?14.1 28.9 25.7 ?11.2
8 12 212.1 37.2 31.8 ?14.4 26.9 24.5 ?8.9
9 10 49.4 23.9 23.0 ?4.0 17.3 21.9 26.8
10 8 331 43.7 33.0 ?24.5 39.2 27.2 ?30.7
11 8 32.6 67.6 51.3 ?24.1 35.9 46.3 28.8
12 4 82.7 62.0 28.4 ?54.2 44.6 19.6 ?56.0
Tab.4 Comparison of VOCs volume fraction for rainy and non-rainy days
Fig.8 Seasonal and annual wind roses in Hangzhou colored by VOCs volume fractions
Fig.9 Seasonal changes of VOCs volume fraction of wind speed under different dominated wind direction
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