Junyu Zheng

Speciated VOC emission inventory and spatial patterns of ozone formation potential in the Pearl River Delta, China.

The Pearl River Delta region (PRD) of China has long suffered from severe ground-level ozone pollution. Knowledge of the sources of volatile organic compounds (VOCs) is essential for ozone chemistry. In this work, a speciated VOC emission inventory was established on the basis of updated emissions and local VOC source profiles. The top 10 species, in terms of ozone formation potentials (OFPs), consisted of isoprene, mp-xylene, toluene, ethylene, propene, o-xylene, 1,2,4-trimethylbenzene, 2-methyl-2-butene, 1-butene, and alpha-pinene. These species contributed only 35.9% to VOCs emissions but accounted for 64.1% of the OFP in the region. The spatial patterns of the VOC source inventory agreed well with city-based source apportionment results, especially for vehicle emissions and industry plus VOC product-related emissions. Mapping of the OFPs and measured ozone concentrations indicated that the formation of higher ozone in the south and southeast of the PRD region differed from that in the Conghua area, a remote area in the north of the PRD. We recommend that the priorities for the control of VOC sources include motorcycles, gasoline vehicles, and solvent use because of their larger OFP contributions.

Speciated OVOC and VOC emission inventories and their implications for reactivity-based ozone control strategy in the Pearl River Delta region, China

The increasing ground-ozone (O3) levels, accompanied by decreasing SO2, NO2, PM10 and PM2.5 concentrations benefited from air pollution control measures implemented in recent years, initiated a serious challenge to control Volatile Organic Compound (VOC) emissions in the Pearl River Delta (PRD) region, China. Speciated VOC emission inventory is fundamental for estimating Ozone Formation Potentials (OFPs) to identify key reactive VOC species and sources in order to formulate efficient O3 control strategies. With the use of the latest bulk VOC emission inventory and local source profiles, this study developed the PRD regional speciated Oxygenated Volatile Organic Compound (OVOC) and VOC emission inventories to identify the key emission-based and OFP-based VOC sources and species. Results showed that: (1) Methyl alcohol, acetone and ethyl acetate were the major constituents in the OVOC emissions from industrial solvents, household solvents, architectural paints and biogenic sources; (2) from the emission-based perspective, aromatics, alkanes, OVOCs and alkenes made up 39.2%, 28.2%, 15.9% and 10.9% of anthropogenic VOCs; (3) from the OFP-based perspective, aromatics and alkenes become predominant with contributions of 59.4% and 25.8% respectively; (4) ethene, m/p-xylene, toluene, 1,2,4-trimethyl benzene and other 24 high OFP-contributing species were the key reactive species that contributed to 52% of anthropogenic emissions and up to 80% of OFPs; and (5) industrial solvents, industrial process, gasoline vehicles and motorcycles were major emission sources of these key reactive species. Policy implications for O3 control strategy were discussed. The OFP cap was proposed to regulate VOC control policies in the PRD region due to its flexibility in reducing the overall OFP of VOC emission sources in practice.

Establishing a conceptual model for photochemical ozone pollution in subtropical Hong Kong

Abstract Photochemical ozone (O3) formation is related to its precursors and meteorological conditions. A conceptual model of O3 air pollution is developed based on the analysis of data obtained at Tung Chung (TC) in Hong Kong. By comparing meteorological parameters between O3 and non-O3 episode days, it was found that high temperatures, strong solar radiation, low wind speeds and relative humidity, northeasterly and/or northwesterly prevailing winds were favorable for the O3 formation, while tropical cyclones were most conducive to the occurrence of O3 episodes. Backward trajectories simulation and graphical illustration of O3 pollution suggested that super-regional (i.e. central and eastern China) and regional (i.e. Pearl River Delta, southern China) transport was another factor that contributed to high O3 levels in Hong Kong. The photochemical O3 formation, generally VOC-limited in Hong Kong, was controlled by a small number of volatile organic compounds (VOCs). Furthermore, the positive matrix factorization (PMF) simulation suggested that solvent usage and vehicular emissions are the major contributors to ambient VOCs in Hong Kong. Finally, this paper presents recommendations for further O3 research and implementation of O3 control strategies.

A refined 2010-based VOC emission inventory and its improvement on modeling regional ozone in the Pearl River Delta Region, China.

Accurate and gridded VOC emission inventories are important for improving regional air quality model performance. In this study, a four-level VOC emission source categorization system was proposed. A 2010-based gridded Pearl River Delta (PRD) regional VOC emission inventory was developed with more comprehensive source coverage, latest emission factors, and updated activity data. The total anthropogenic VOC emission was estimated to be about 117.4 × 10(4)t, in which on-road mobile source shared the largest contribution, followed by industrial solvent use and industrial processes sources. Among the industrial solvent use source, furniture manufacturing and shoemaking were major VOC emission contributors. The spatial surrogates of VOC emission were updated for major VOC sources such as industrial sectors and gas stations. Subsector-based temporal characteristics were investigated and their temporal variations were characterized. The impacts of updated VOC emission estimates and spatial surrogates were evaluated by modeling O₃ concentration in the PRD region in the July and October of 2010, respectively. The results indicated that both updated emission estimates and spatial allocations can effectively reduce model bias on O₃ simulation. Further efforts should be made on the refinement of source classification, comprehensive collection of activity data, and spatial-temporal surrogates in order to reduce uncertainty in emission inventory and improve model performance.

Ambient Ozone Control in a Photochemically Active Region: Short-Term Despiking or Long-Term Attainment?

China has made significant progress decreasing the ambient concentrations of most air pollutants, but ozone (O3) is an exception. O3 mixing ratios during pollution episodes are far higher than the national standard in the Pearl River Delta (PRD), thus greater evidence-based control efforts are needed for O3 attainment. By using a validated O3 modeling system and the latest regional emission inventory, this study illustrates that control strategies for short-term O3 despiking and long-term attainment in the PRD may be contradictory. VOC-focused controls are more efficient for O3 despiking in urban and industrial areas, but significant NOx emission reductions and a subsequent transition to a NOx-limited regime are required for O3 attainment. By tracking O3 changes along the entire path toward long-term attainment, this study recommends to put a greater focus on NOx emission controls region-wide. Parallel VOC reductions around the Nansha port are necessary in summertime and should be extended to the urban and industrial areas in fall with a flexibility to be strengthened on days forecasted to have elevated O3. Contingent VOC-focused controls on top of regular NOx-focused controls would lay the groundwork for striking a balance between short-term despiking and long-term attainment of O3 concentrations in the PRD.

Road-Network-Based Spatial Allocation of On-Road Mobile Source Emissions in the Pearl River Delta Region, China, and Comparisons with Population-Based Approach

Abstract Gridded air pollutant emission inventories are prerequisites for using air quality models to assess air pollution control strategies and predict air quality. A precise gridded emission inventory will help improve the accuracy of air quality simulation. Mobile source emissions are one of the major contributors to volatile organic compound (VOC) and nitrogen oxide (NOx) pollutants, the precursors of ozone formation. However, because of the complexity of road networks and variations in traffic flows at different road types and locations, spatial allocation of emissions from mobile sources into grid cells is challenging. This paper proposes a new methodological framework, named as “the road-network-based approach,” for spatially allocating regional mobile source emission inventories. The new approach utilizes the Geographic Information System (GIS)-based road network information and road-types-based traffic flow data to provide spatial surrogates for allocating Pearl River Delta (PRD) regional mobile source emission inventories. The results show that the new approach provides reasonable spatial distributions of mobile source emissions, and the distributions are in good agreement with PRD regional on-road emission line sources. Comparisons between using the population-based and the new road-network-based approaches are made. The air quality modeling results indicate that the new approach can obviously improve model predictions with increasing accuracy in mobile source emission allocations. Means of choosing appropriate approaches for spatially allocating regional mobile source emissions are discussed.

An AIS-based high-resolution ship emission inventory and its uncertainty in Pearl River Delta region, China

Ship emissions contribute significantly to air pollution and impose health risks to residents along the coastal area. By using the refined data from the Automatic Identification System (AIS), this study developed a highly resolved ship emission inventory for the Pearl River Delta (PRD) region, China, home to three of ten busiest ports in the world. The region-wide SO2, NOX, CO, PM10, PM2.5, and VOC emissions in 2013 were estimated to be 61,484, 103,717, 10,599, 7155, 6605, and 4195t, respectively. Ocean going vessels were the largest contributors of the total emissions, followed by coastal vessels and river vessels. In terms of ship type, container ship was the leading contributor, followed by conventional cargo ship, dry bulk carrier, fishing ship, and oil tanker. These five ship types accounted for >90% of total emissions. The spatial distributions of emissions revealed that the key emission hot spots all concentrated within the newly proposed emission control area (ECA) and ship emissions within ECA covered >80% of total ship emissions in the PRD, highlighting the importance of ECA in emissions reduction in the PRD. The uncertainties of emission estimates of pollutants were quantified, with lower bounds of -24.5% to -21.2% and upper bounds of 28.6% to 33.3% at 95% confidence intervals. The lower uncertainties in this study highlighted the powerfulness of AIS data in improving ship emission estimates. The AIS-based bottom-up methodology can be used for developing and upgrading ship emission inventory and formulating effective control measures on ship emissions in other port regions wherever possible.

Potential sources of nitrous acid (HONO) and their impacts on ozone : a WRF-Chem study in a polluted subtropical region

Current chemical transport models commonly undersimulate the atmospheric concentration of nitrous acid (HONO), which plays an important role in atmospheric chemistry, due to the lack or inappropriate representations of some sources in the models. In the present study, we parameterized up-to-date HONO sources into a state-of-the-art three-dimensional chemical transport model (Weather Research and Forecasting model coupled with Chemistry: WRF-Chem). These sources included (1) heterogeneous reactions on ground surfaces with the photoenhanced effect on HONO production, (2) photoenhanced reactions on aerosol surfaces, (3) direct vehicle and vessel emissions, (4) potential conversion of NO2 at the ocean surface, and (5) emissions from soil bacteria. The revised WRF-Chem was applied to explore the sources of the high HONO concentrations (0.45–2.71 ppb) observed at a suburban site located within complex land types (with artificial land covers, ocean, and forests) in Hong Kong. With the addition of these sources, the revised model substantially reproduced the observed HONO levels. The heterogeneous conversions of NO2 on ground surfaces dominated HONO sources contributing about 42% to the observed HONO mixing ratios, with emissions from soil bacterial contributing around 29%, followed by the oceanic source (~9%), photochemical formation via NO and OH (~6%), conversion on aerosol surfaces (~3%), and traffic emissions (~2%). The results suggest that HONO sources in suburban areas could be more complex and diverse than those in urban or rural areas and that the bacterial and/or ocean processes need to be considered in HONO production in forested and/or coastal areas. Sensitivity tests showed that the simulated HONO was sensitive to the uptake coefficient of NO2 on the surfaces. Incorporation of the aforementioned HONO sources significantly improved the simulations of ozone, resulting in increases of ground-level ozone concentrations by 6–12% over urban areas in Hong Kong and the Pearl River Delta region. This result highlights the importance of accurately representing HONO sources in simulations of secondary pollutants over polluted regions.

Sector-based VOCs emission factors and source profiles for the surface coating industry in the Pearl River Delta region of China

Accurate depiction of VOCs emission characteristics is essential for the formulation of VOCs control strategies. As one of the continuous efforts in improving VOCs emission characterization in the Pearl River Delta (PRD) region, this study targeted on surface coating industry, the most important VOCs emission sources in the PRD. Sectors in analysis included shipbuilding coating, wood furniture coating, metal surface coating, plastic surface coating, automobile coating and fabric surface coating. Sector-based field measurement was conducted to characterize VOCs emission factors and source profiles in the PRD. It was found that the raw material-based VOCs emission factors for these six sectors ranged from 0.34 to 0.58kg VOCs per kg of raw materials (kg·kg-1) while the emission factors based on the production yield varied from 0.59kg to 13.72t VOCs for each production manufactured. VOCs emission factors of surface coating industry were therefore preferably calculated based on raw materials with low uncertainties. Source profiles differed greatly among different sectors. Aromatic was the largest group for shipbuilding coating, wood furniture coating, metal surface coating and automobile coating while the oxygenated VOCs (OVOCs) were the most abundant in the plastic and fabric surface coating sectors. The major species of aromatic VOCs in each of these six sectors were similar, mainly toluene and m/p-xylene, while the OVOCs varied among the different sectors. VOCs profiles in the three processes of auto industry, i.e., auto coating, auto drying and auto repairing, also showed large variations. The major species in these sectors in the PRD were similar with other places but the proportions of individual compounds were different. Some special components were also detected in the PRD region. This study highlighted the importance of updating local source profiles in a comprehensive and timely manner.

A New Combined Stepwise-Based High-Order Decoupled Direct and Reduced-Form Method To Improve Uncertainty Analysis in PM2.5 Simulations

The traditional reduced-form model (RFM) based on the high-order decoupled direct method (HDDM), is an efficient uncertainty analysis approach for air quality models, but it has large biases in uncertainty propagation due to the limitation of the HDDM in predicting nonlinear responses to large perturbations of model inputs. To overcome the limitation, a new stepwise-based RFM method that combines several sets of local sensitive coefficients under different conditions is proposed. Evaluations reveal that the new RFM improves the prediction of nonlinear responses. The new method is applied to quantify uncertainties in simulated PM2.5 concentrations in the Pearl River Delta (PRD) region of China as a case study. Results show that the average uncertainty range of hourly PM2.5 concentrations is -28% to 57%, which can cover approximately 70% of the observed PM2.5 concentrations, while the traditional RFM underestimates the upper bound of the uncertainty range by 1-6%. Using a variance-based method, the PM2.5 boundary conditions and primary PM2.5 emissions are found to be the two major uncertainty sources in PM2.5 simulations. The new RFM better quantifies the uncertainty range in model simulations and can be applied to improve applications that rely on uncertainty information.