Wang Xiaoliang, Khlystov Andrey, Ho Kin-Fai, Campbell Dave, Chow Judith C, Kohl Steven D, Watson John G, Lee Shun-Cheng Frank, Chen Lung-Wen Antony, Lu Minggen, Ho Steven Sai Hang
Desert Research Institute, Reno, Nevada, United States.
The Chinese University of Hong Kong, China.
Res Rep Health Eff Inst. 2019 Mar;2019(199):5-52.
Motor vehicle exhaust is an important source of air pollutants and greenhouse gases. Concerns over the health and climate effects of mobile-source emissions have prompted worldwide efforts to reduce vehicle emissions. Implementation of more stringent emission standards have driven advances in vehicle, engine, and exhaust after-treatment technologies as well as fuel formulations. On the other hand, vehicle numbers and travel distances have been increasing because of population and economic growth and changes in land use. These factors have resulted in changes to the amount and chemical composition of vehicle emissions.
Roadway tunnel studies are a practical way to characterize real-world emissions from the on-road vehicle fleet in an environment isolated from other combustion pollution sources. Measurements in the same tunnel over time allow evaluation of vehicle emission changes and the effectiveness of emission reduction measures. Tunnel studies estimate the impacts of vehicle emissions on air quality and traffic-related exposures, generate source profile inputs for receptor-oriented source apportionment models, provide data to evaluate emission models, and serve as a baseline for future comparisons.
The present study characterized motor vehicle emission factors and compositions in two roadway tunnels that were first studied over a decade ago. The specific aims were to (1) quantify current fleet air pollutant emission factors, (2) evaluate emission change over time, (3) establish source profiles for volatile organic compounds (VOCs) and particulate matter ≤2.5 μm in aerodynamic diameter (PM), (4) estimate contributions of fleet components and non-tailpipe emissions to VOCs and PM, and (5) evaluate the performance of the latest versions of mobile-source emission models (i.e., the EMission FACtors vehicle emission model used in Hong Kong [EMFAC-HK] and the MOtor Vehicle Emission Simulator used in the United States [MOVES]).
Measurements were conducted in the Shing Mun Tunnel (SMT) in Hong Kong and the Fort McHenry Tunnel (FMT) in Baltimore, Maryland, in the United States, representing the different fleet compositions, emission controls, fuels, and near-road exposure levels found in Hong Kong and the United States. These tunnels have extensive databases acquired in 2003-2004 for the SMT and 1992 for the FMT. The SMT sampling was conducted during the period from 1/19/2015 to 3/31/2015, and the FMT sampling occurred during the periods from 2/8/2015 to 2/15/2015 (winter) and 7/31/2015 to 8/7/2015 (summer). Concentrations of criteria pollutants (e.g., carbon monoxide [CO], nitrogen oxides [NOx], and particulate matter [PM]) were measured in real time, and integrated samples of VOCs, carbonyls, polycyclic aromatic hydrocarbons (PAHs), and PM were collected in canisters and sampling media for off-line analyses. Emission factors were calculated from the tunnel measurements and compared with previous studies to evaluate emission changes over time. Emission contributions by different vehicle types were assessed by source apportionment modeling or linear regression. Vehicle emissions were modeled by EMFAC-HK version 3.3 and MOVES version 2014a for the SMT and the FMT, respectively, and compared with measured values. The influences of vehicle fleet composition and environmental parameters (i.e., temperature and relative humidity) on emissions were evaluated.
In the SMT, emissions of PM, sulfur dioxide (SO), and total non-methane hydrocarbons (NMHCs) markedly decreased from 2003-2004 to 2015: SO and PM were reduced by ~80%, and total NMHCs was reduced by ~44%. Emission factors of ethene and propene, key tracers for diesel vehicle (DV) emissions, decreased by ~65%. These reductions demonstrate the effectiveness of control measures, such as the implementation of low-sulfur fuel regulations and the phasing out of older DVs. However, the emission factors of isobutane and -butane, markers for liquefied petroleum gas (LPG), increased by 32% and 17% between 2003-2004 and 2015, respectively, because the number of LPG vehicles increased. Nitrogen dioxide (NO) to NOx volume ratios increased between 2003-2004 and 2015, indicating an increased NO fraction in primary exhaust emissions. Although geological mineral concentrations were similar between the 2003-2004 and 2015 studies, the contribution of geological materials to PM increased from 2% in 2003-2004 to 5% in 2015, signifying the continuing importance of non-tailpipe PM emissions as tailpipe emissions decrease. Emissions of CO, ammonia (NH), nitric oxide (NO), NO, and NOx, as well as carbonyls and PAHs in the SMT did not show statistically significant (at < 0.05 based on Student's -test) decreases from 2003-2004 to 2015. The reason for this is not clear and requires further investigation.
A steady decrease in emissions of all measured pollutants during the past 23 years has been observed from tunnel studies in the United States, reflecting the effect of emission standards and new technologies that were introduced during this period. Emission reductions were more pronounced for the light-duty (LD) fleet than for the heavy-duty (HD) fleet. In comparison with the 1992 FMT study, the 2015 FMT study demonstrated marked reductions in LD emissions for all pollutants: emission factors for naphthalene were reduced the most, by 98%; benzene, toluene, ethylbenzene, and xylene (BTEX), by 94%; CO, NMHCs, and NOx, by 87%; and aldehydes by about 71%. Smaller reductions were observed for HD emission factors: naphthalene emissions were reduced by 95%, carbonyl emissions decreased by about 75%, BTEX by 60%, and NOx 58%.
The 2015 fleet-average emission factors were higher in the SMT for CO, NOx, and summer PM than those in the FMT. The higher CO emissions in the SMT were possibly attributable to a larger fraction of motorcycles and LPG vehicles in the Hong Kong fleet. DVs in Hong Kong and the United States had similar emission factors for NOx. However, the non-diesel vehicles (NDVs), particularly LPG vehicles, had higher emission factors than those of gasoline cars, contributing to higher NOx emissions in the SMT. The higher PM emission factors in the SMT were probably attributable to there being more double-deck buses in Hong Kong.
In both tunnels, PAHs were predominantly in the gas phase, with larger (four and more aromatic rings) PAHs mostly in the particulate phase. Formaldehyde, acetaldehyde, crotonaldehyde, and acetone were the most abundant carbonyl compounds in the SMT. In the FMT, the most abundant carbonyls were formaldehyde, acetone, acetaldehyde, and propionaldehyde. HD vehicles emitted about threefold more carbonyl compounds than LD vehicles did. In the SMT, the NMHC species were enriched with marker species for LPG (e.g., -butane, isobutane, and propane) and gasoline fuel vapor (e.g., toluene, isopentane, and -xylene), indicating evaporative losses. Source contributions to SMT PM mass were diesel exhaust (51.5 ± 1.8%), gasoline exhaust (10.0 ± 0.8%), LPG exhaust (5.0 ± 0.5%), secondary sulfate (19.9 ± 1.0%), secondary nitrate (6.3 ± 0.9%), and road dust (7.3 ± 1.3%). In the FMT, total NMHC emissions were 14% and 8% higher in winter than in summer for LD and HD vehicles, respectively. Elemental carbon (EC) and organic carbon (OC) were the major constituents of tunnel PM. De-icing salt contributions to PM were observed in the FMT in winter.
Emission estimates by the EMFAC-HK agreed with SMT measurements for CO; the modeled emission factors for CO, NOx, and NMHCs were 1.5, 1.6, and 2.2 times the measurements, respectively; and the modeled emission factor for PM was 61% of the measured value in 2003. The EMFAC-HK estimates and SMT measurements for 2015 differed by less than 35%. The MOVES2014a model generally overestimated emissions of most of the pollutants measured in the FMT. No pollutants were significantly underestimated. The largest overestimation was observed for emissions measured during HD-rich driving conditions in winter.
Significant reductions in SO and PM emissions between 2003 and 2015 were observed in the SMT, indicating the effectiveness of control measures on these two pollutants. The total NMHC emissions in the SMT were reduced by 44%, although isobutane and -butane emissions increased because of the increase in the size of the LPG fleet. No significant reductions were observed for CO and NOx, results that differed from those for roadside ambient concentrations, emission inventory estimates, and EMFAC-HK estimates. In contrast, there was a steady decrease in emissions of most pollutants in the tunnels in the United States.
机动车尾气是空气污染物和温室气体的重要来源。对移动源排放所产生的健康和气候影响的担忧促使全球各国努力减少车辆排放。实施更严格的排放标准推动了车辆、发动机和尾气后处理技术以及燃料配方的进步。另一方面,由于人口增长、经济发展和土地利用变化,车辆数量和行驶里程一直在增加。这些因素导致了车辆排放的数量和化学成分发生变化。
巷道隧道研究是一种在与其他燃烧污染源隔离的环境中表征道路车辆实际排放的实用方法。随着时间的推移在同一隧道内进行测量,可以评估车辆排放的变化以及减排措施的有效性。隧道研究可以估算车辆排放对空气质量和与交通相关暴露的影响,为面向受体的源解析模型生成源成分谱输入,提供数据以评估排放模型,并作为未来比较的基线。
本研究对两条巷道隧道中的机动车排放因子和成分进行了表征,这两条隧道在十多年前首次进行了研究。具体目标是:(1)量化当前车队的空气污染物排放因子;(2)评估随时间的排放变化;(3)建立挥发性有机化合物(VOCs)和空气动力学直径≤2.5μm的颗粒物(PM)的源成分谱;(4)估算车队组成部分和非尾气排放对VOCs和PM的贡献;(5)评估最新版本的移动源排放模型(即香港使用的排放因子车辆排放模型[EMFAC - HK]和美国使用的机动车排放模拟器[MOVES])的性能。
测量工作分别在美国马里兰州巴尔的摩的麦克亨利堡隧道(FMT)和中国香港的城门隧道(SMT)中进行,这两条隧道代表了香港和美国不同的车队组成、排放控制、燃料以及道路附近暴露水平。这些隧道拥有在2003 - 2004年(SMT)和1992年(FMT)获取的广泛数据库。SMT的采样在2015年1月19日至3月31日期间进行,FMT的采样在2015年2月8日至2月15日(冬季)和2015年7月31日至8月7日(夏季)期间进行。实时测量了标准污染物(如一氧化碳[CO]、氮氧化物[NOx]和颗粒物[PM])的浓度,并在采样罐和采样介质中收集了VOCs、羰基化合物、多环芳烃(PAHs)和PM的综合样本用于离线分析。根据隧道测量结果计算排放因子,并与先前的研究进行比较,以评估随时间的排放变化。通过源解析建模或线性回归评估不同车辆类型的排放贡献。分别使用EMFAC - HK版本3.3和MOVES版本2014a对SMT和FMT的车辆排放进行建模,并与测量值进行比较。评估了车队组成和环境参数(即温度和相对湿度)对排放的影响。
在SMT中,从2003 - 2004年到2015年,PM、二氧化硫(SO)和总非甲烷碳氢化合物(NMHCs)的排放量显著下降:SO和PM减少了约8