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化学进展 2023, Vol. 35 Issue (1): 177-188 DOI: 10.7536/PC220605 前一篇   

• 综述 •

机动车尾气二次有机气溶胶生成研究

国纪良, 彭剑飞*(), 宋爱楠, 张进生, 杜卓菲*(), 毛洪钧   

  1. 天津市城市交通污染防治研究重点实验室 南开大学环境科学与工程学院 天津 300071
  • 收稿日期:2022-06-08 修回日期:2022-08-01 出版日期:2023-01-24 发布日期:2022-09-19
  • 作者简介:

    彭剑飞 北京大学学士、博士,美国德州农机大学博士后,2020年5月任南开大学环境科学与工程学院教授。主要从事大气二次颗粒物生成机制、交通源排放与控制、黑碳颗粒物老化及环境效应等领域研究,以第一或通讯作者在PNAS、Environ. Sci. Technol.、Atmos. Chem. Phys.等期刊发表文章16篇,SCI引用超过3600次。

    杜卓菲 北京大学博士,南开大学助理研究员。主要研究方向为交通源的排放与转化、黑碳气溶胶老化及效应,以第一或通讯作者在Atmos. Chem. Phys.、J. Clean. Prod.等SCI期刊发表多篇文章。

  • 基金资助:
    国家自然科学基金项目(42175123); 国家自然科学基金项目(42107125); ,天津市自然科学基金项目(20JCYBJC01270); 天津市研究生科研创新项目(2021YJSS013)
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Studies on the Formation of Secondary Organic Aerosol from Vehicle Exhaust

Jiliang Guo, Jianfei Peng(), Ainan Song, Jinsheng Zhang, Zhuofei Du(), Hongjun Mao   

  1. Tianjin Key Laboratory of Urban Transport Emission Research, College of Environmental Science and Engineering, Nankai University, Tianjin 300071, China
  • Received:2022-06-08 Revised:2022-08-01 Online:2023-01-24 Published:2022-09-19
  • Contact: *e-mail: pengjianfei@nankai.edu.cn (Jianfei Peng); duzhuofei11235@nankai.edu.cn (Zhuofei Du)
  • Supported by:
    National Natural Science Foundation of China(42175123); National Natural Science Foundation of China(42107125); Natural Science Foundation of Tianjin(20JCYBJC01270); Tianjin Research Innovation Project for Postgraduate Students(2021YJSS013)

二次有机气溶胶(SOA)是大气细颗粒物(PM2.5)的重要组分,对大气能见度、公众健康以及区域或全球气候变化具有重要影响。在城市地区,机动车尾气排放的气态前体物在大气中氧化产生高浓度SOA,是城市空气质量下降的重要因素。本文综述了近些年机动车尾气SOA生成的相关研究成果,重点关注关键前体物的识别与排放表征、SOA生成特征、演化过程与影响因素,对比了不同研究得到的机动车SOA生成因子的差异,并提出新测量技术、新反应机制和新参数化方案将是未来研究重点关注的方向。

关键词： 机动车尾气, 二次有机气溶胶, 半/中等挥发性有机物, 老化过程, 影响因素

Secondary organic aerosol (SOA) is an important component of fine particulate matter (PM2.5), which significantly impacts on atmospheric visibility, human health and regional/global climate change. In urban air, high level of SOA is formed from the atmospheric oxidation of gaseous organic precursors emitted from vehicles, becoming an important factor for the decline of urban air quality. This review summarizes recent studies on the SOA formation from vehicle exhaust, focusing on the identification of key precursors and their emission characteristics, as well as SOA formation, evolution, and influencing factors. In addition, SOA production factors are compared among studies. New measuring techniques, new mechanisms and new parametric method will be the key research direction in the future.

Contents

1 Introduction

2 Identification of SOA precursors from vehicle exhaust and their emission characteristics

2.1 Measurement methods

2.2 Emission characteristics and influencing factors

3 Laboratory simulation of SOA formation from vehicle exhaust

3.1 Smog chamber and flow tube experiments

3.2 Influencing factors of SOA formation

3.3 Evolution and product composition of SOA

3.4 Model simulation of SOA formation

4 Conclusion and prospect

Key words: vehicle exhaust, secondary organic aerosol, semi/intermediate volatility organic compounds, aging process, influencing factor
()
图1 PMCAMx模型在四种预测情景下的OA浓度图: (A)POA不挥发的传统模型,(B)POA具有半挥发性但不反应,(C)POA能够被OH自由基氧化,(D)向模型中加入S/IVOCs,生成大量SOA[17]
Fig. 1 Maps of predicted ground-level OA concentrations for four PMCAMx simulations:(A) A traditional model with nonvolatile POA emissions, (B) POA emissions are volatile but not reactive, (C) POA are also aged by OH, (D) Add additional S/IVOCs emissions to the model which create a considerable amount of regional SOA[17]. Copyright ? 2007, The American Association for the Advancement of Science.
表1 尾气中IVOCs的排放因子
Table 1 IVOCs emission factors of vehicle exhaust
Operation conditions IVOCs EF(mg· kg·fuel-1) ref
Gasoline Vehicle/engine
Pre-LEV Cold start UC cycle 160.6 27
LEV Ⅰ 48.5
LEV Ⅱ 22.4
Tier 0 Cold start UC cycle 54.4 47
LEV Ⅰ 40.6
LEV Ⅱ 16.5
ULEV 18.4
SULEV 4
Tunnle text — 244 48
239.5 32
Euro 5 CLTC、WLTC 12.1~226.3 23
Diesel Vehicle/engine
HDDV UDDS DPF+DOC 24.1 43
none 705.9
Creep+Idle DPF+SCR+DOC 104.9
DPF+DOC 1066.9
none 4089.2
Hi-Cruise none 705.8
MDDV Cold UC DOC 767.8
none 631.3
Euro 5 diesel engine No aftertreatment HS/HL 154 36
LS/LL 97.9
HS/LL 51.2
DOC HS/LL 101
DOC+DPF HS/HL 68.2
LS/LL 55.3
HS/LL 25.9
Light-duty diesel engine Cold stat 9296 49
Cold loaded 2902
WIFL 1438
Tunnle text — 984.9 32
1107 48
Off-road Engine/ Constuction
TRU 4-Mode Cycle C 691.1 43
2-stock SORE CARB procedures 6064 27
4-stock SORE 1149
road roller Idle 1570.5 50
Moving 1038.9
Working 549.1
motor grader Idle 879.8
Moving 608.5
Working 305.9
图2 中、美地区机动车尾气SOA生成因子: a)不同生产年份或排放标准的汽油车尾气SOA生成因子,OH暴露量=(3~5)×106 molecules cm-3·h,b)重型或中型柴油车尾气SOA生成因子,OH暴露量= 2×106 ~ 2×107 molecules cm-3·h
Fig. 2 SOA production factor of vehicle exhaust in China and US. a) SOA production factor of gasoline vehicle exhaust with different model years or emission standards, OH exposure = (3~5)×106 molecules cm-3·h, b)SOA production factor of heavy or medium duty diesel vehicle exhaust, OH exposure= 2×106~2×107 molecules cm-3·h.
图3 a)SOA中m/z 43与m/z 44信号对总有机信号的占比(f43 vs f44)和Ng提出的三角图[83]; b) 尾气SOA老化的Van-Krevelen图[16,67,80,82]
Fig. 3 a) Fractions of entire organic signals at m/z 43 and m/z 44(f43 vs f44)from exhaust derived SOA as well as an Ng triangle plot[83]; b) Van-Krevelen diagram of SOA from vehicle exhaust[16,67,80,82]
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