Decades of air quality improvements have substantially reduced the motor vehicle emissions of volatile organic compounds (VOCs). Today, volatile chemical products (VCPs) are responsible for half of the petrochemical VOCs emitted in major urban areas. We show that VCP emissions are ubiquitous in US and European cities and scale with population density. We report significant VCP emissions for New York City (NYC), including a monoterpene flux of 14.7 to 24.4 kg ⋅ d−1 ⋅ km−2 from fragranced VCPs and other anthropogenic sources, which is comparable to that of a summertime forest. Photochemical modeling of an extreme heat event, with ozone well in excess of US standards, illustrates the significant impact of VCPs on air quality. In the most populated regions of NYC, ozone was sensitive to anthropogenic VOCs (AVOCs), even in the presence of biogenic sources. Within this VOC-sensitive regime, AVOCs contributed upwards of ∼20 ppb to maximum 8-h average ozone. VCPs accounted for more than 50% of this total AVOC contribution. Emissions from fragranced VCPs, including personal care and cleaning products, account for at least 50% of the ozone attributed to VCPs. We show that model simulations of ozone depend foremost on the magnitude of VCP emissions and that the addition of oxygenated VCP chemistry impacts simulations of key atmospheric oxidation products. NYC is a case study for developed megacities, and the impacts of VCPs on local ozone are likely similar for other major urban regions across North America or Europe. Significance Recent work in Los Angeles has shown that urban volatile organic compound (VOC) emissions from consumer and industrial products—termed volatile chemical products (VCPs)—are now an important source of ozone precursors. Using advancements in VOC instrumentation, we show that VCP emissions are ubiquitous in urban regions and can be identified via unique VOC fingerprints. Through detailed modeling, we show that VCPs are as important to ozone production as fossil fuel VOCs and that the chemistry of VCPs can have significant impacts on model simulations of key atmospheric processes. Consequently, air quality models must be updated to account for both the emissions and atmospheric chemistry of VCPs in order to capture their full impact on urban air quality.
The largest uncertainty in the radiative forcing of climate change over the industrial era is that due to aerosols, a substantial fraction of which is the uncertainty associated with scattering and absorption of shortwave (solar) radiation by anthropogenic aerosols in cloud-free conditions (IPCC, 2001). Quantifying and reducing the uncertainty in aerosol influences on climate is critical to understanding climate change over the industrial period and to improving predictions of future climate change for assumed emission scenarios. Measurements of aerosol properties during major field campaigns in several regions of the globe during the past decade are contributing to an enhanced understanding of atmospheric aerosols and their effects on light scattering and climate. The present study, which focuses on three regions downwind of major urban/population centers (North Indian Ocean (NIO) during INDOEX, the Northwest Pacific Ocean (NWP) during ACE-Asia, and the Northwest Atlantic Ocean (NWA) during ICARTT), incorporates understanding gained from field observations of aerosol distributions and properties into calculations of perturbations in radiative fluxes due to these aerosols. This study evaluates the current state of observations and of two chemical transport models (STEM and MOZART). Measurements of burdens, extinction optical depth (AOD), and direct radiative effect of aerosols (DRE – change in radiative flux due to total aerosols) are used as measurement-model check points to assess uncertainties. In-situ measured and remotely sensed aerosol properties for each region (mixing state, mass scattering efficiency, single scattering albedo, and angular scattering properties and their dependences on relative humidity) are used as input parameters to two radiative transfer models (GFDL and University of Michigan) to constrain estimates of aerosol radiative effects, with uncertainties in each step propagated through the analysis. Constraining the radiative transfer calculations by observational inputs increases the clear-sky, 24-h averaged AOD (34±8%), top of atmosphere (TOA) DRE (32±12%), and TOA direct climate forcing of aerosols (DCF – change in radiative flux due to anthropogenic aerosols) (37±7%) relative to values obtained with "a priori" parameterizations of aerosol loadings and properties (GFDL RTM). The resulting constrained clear-sky TOA DCF is −3.3±0.47, −14±2.6, −6.4±2.1 Wm−2 for the NIO, NWP, and NWA, respectively. With the use of constrained quantities (extensive and intensive parameters) the calculated uncertainty in DCF was 25% less than the "structural uncertainties" used in the IPCC-2001 global estimates of direct aerosol climate forcing. Such comparisons with observations and resultant reductions in uncertainties are essential for improving and developing confidence in climate model calculations incorporating aerosol forcing.
22 September 2005 in Journal of Geophysical Research: Atmospheres
The Planetary Boundary Layer Height (PBLH) plays an important role in the formation and development of air pollution events. Particulate Matter is one of major pollutants in China. Here, we present the characteristics of PBLH through three-methods of Lidar data inversion and show the correlation between the PBLH and the PM2.5 (PM2.5 with the diameter 75 μg/m3 and the PM2.5 < 35 μg/m3 in daytime, respectively. The low PBLH often occurs with condition of the low wind speed and high relative humidity, which will lead to high PM2.5 concentration and the low visibility. On the other hand, the stability of PBL is enhanced by high PM concentration and low visibility.
14 September 2021 in Journal of Geophysical Research: Atmospheres
Stratospheric intrusions are an important source of ozone (O3) in the troposphere. In this study, 17 years of O3 sounding data from the Hong Kong Observatory with a weekly sampling frequency are analyzed to identify stratospheric intrusions and quantify their impact on O3 enhancement events in springtime from 2004 to 2020. 24.7% of O3 enhancement events are related to stratospheric intrusion whereas 31.7% of intrusions lead to the enhancement of O3 in the lower troposphere. Occurrences of stratospheric intrusion in springtime are closely related to tropopause folding and tropospheric convective activities in subtropical regions. The Weather Research and Forecasting model coupled with Chemistry simulations are conducted with the integrated process analysis to quantify the impact of stratospheric intrusions on the enhancement of O3 in the lower free troposphere as well as near the surface under different synoptic patterns. Synoptic patterns associated with stratospheric intrusion‐driving O3 enhancements are classified into two categories: Saddle Point (“S”) and Cold Front (“F”). While downward transport of O3‐enriched air from the enhancement layer exerts an important impact on surface O3 for synoptic pattern “S,” the impact on surface O3 is limited for surface pattern “F.” The impact of stratospheric intrusions together with entrainment on surface O3 may have a strong indication on the development of effective emission control strategies on surface O3 reduction in Hong Kong.