scholarly journals The significant contribution of HONO to secondary pollutants during a severe winter pollution event in southern China

2019 ◽  
Vol 19 (1) ◽  
pp. 1-14 ◽  
Author(s):  
Xiao Fu ◽  
Tao Wang ◽  
Li Zhang ◽  
Qinyi Li ◽  
Zhe Wang ◽  
...  

Abstract. Nitrous acid (HONO) can strongly affect atmospheric photochemistry in polluted regions through the production of hydroxyl radicals (OHs). In January 2017, a severe pollution episode occurred in the Pearl River Delta (PRD) of China, with maximum hourly PM2.5, ozone, and HONO levels reaching 400 µg m−3, 150 ppb, and 8 ppb, respectively, at a suburban site. The present study investigated the sources and processes generating such high HONO concentrations and the role of HONO chemistry in this severe winter episode. Four recently reported HONO sources were added to the Community Multiscale Air Quality (CMAQ) model, including RH-dependent (relative humidity) and light-enhancing effects on heterogeneous reactions, photolysis of particulate nitrate in the atmosphere, and photolysis of HNO3 and nitrate on surfaces. The revised model reproduced the observed HONO and significantly improved its performance for O3 and PM2.5. The model simulations showed that the heterogeneous generation on surfaces (with RH and light effects) was the largest contributor (72 %) to the predicted HONO concentrations, with the RH-enhancing effects more significant at nighttime and the light-enhancing effects more important in the daytime. The photolysis of total nitrate in the atmosphere and deposited on surfaces was the dominant HONO source during noon and afternoon, contributing above 50 % of the simulated HONO. The HONO photolysis was the dominant contributor to HOx production in this episode. With all HONO sources, the daytime average O3 at the Heshan site was increased by 24 ppb (or 70 %), compared to the simulation results without any HONO sources. Moreover, the simulated mean concentrations of TNO3 (HNO3+ fine particle NO3-) at the Heshan site, which was the key species for this haze formation, increased by about 17 µg m−3 (67 %) due to the HONO chemistry, and the peak enhancement reached 55 µg m−3. This study highlights the key role of HONO chemistry in the formation of winter haze in a subtropical environment.

2018 ◽  
Author(s):  
Xiao Fu ◽  
Tao Wang ◽  
Li Zhang ◽  
Qinyi Li ◽  
Zhe Wang ◽  
...  

Abstract. Nitrous acid (HONO) can strongly affect atmospheric photochemistry in polluted regions through the production of hydroxyl radical (OH). In January 2017, a severe pollution episode occurred in the Pearl River Delta (PRD) of China, with maximum hourly PM2.5, ozone and HONO levels reaching 400 µg/m3, 150 ppb, and 8 ppb, respectively, at a suburban site. The present study investigated the sources/processes generating such high HONO concentrations and the role of HONO chemistry in this severe winter episode. Four recently reported HONO sources were added to the Community Multi-scale Air Quality (CMAQ) model, including RH-dependent and light-enhancing effects on heterogeneous reactions, photolysis of particulate nitrate in the atmosphere, and photolysis of HNO3 and nitrate on surfaces. The revised model reproduced the observed HONO and significantly improved its performance for O3 and PM2.5. The model simulations showed that the heterogeneous generation on surfaces (with RH and light effects) was the largest contributor (72 %) to the predicted HONO concentrations, with the RH-enhancing effects more significant at nighttime and the light-enhancing effects more important in the daytime. The photolysis of total nitrate in the atmosphere and deposited on surfaces was the dominant HONO source during noon and afternoon, contributing above 50 % of the simulated HONO. The HONO photolysis was the dominant contributor to HOX production in this episode. With all HONO sources, the daytime average O3 at Heshan site was increased by 24 ppb (or 70 %), compared to the simulation results without any HONO sources. Moreover, the simulated mean concentrations of TNO3 (HNO3 + fine particle NO3−) at Heshan site, which was the key species for this haze formation, increased by about 17 µg/m3 (67 %) due to the HONO chemistry, and the peak enhancement reached 55 µg/m3. This study highlights the key role of HONO chemistry in the formation of winter haze in a subtropical environment.


2021 ◽  
Vol 4 (1) ◽  
Author(s):  
Wei Du ◽  
Lubna Dada ◽  
Jian Zhao ◽  
Xueshun Chen ◽  
Kaspar R. Daellenbach ◽  
...  

AbstractThe role of new particle formation (NPF) events and their contribution to haze formation through subsequent growth in polluted megacities is still controversial. To improve the understanding of the sources, meteorological conditions, and chemistry behind air pollution, we performed simultaneous measurements of aerosol composition and particle number size distributions at ground level and at 260 m in central Beijing, China, during a total of 4 months in 2015–2017. Our measurements show a pronounced decoupling of gas-to-particle conversion between the two heights, leading to different haze processes in terms of particle size distributions and chemical compositions. The development of haze was initiated by the growth of freshly formed particles at both heights, whereas the more severe haze at ground level was connected directly to local primary particles and gaseous precursors leading to higher particle growth rates. The particle growth creates a feedback loop, in which a further development of haze increases the atmospheric stability, which in turn strengthens the persisting apparent decoupling between the two heights and increases the severity of haze at ground level. Moreover, we complemented our field observations with model analyses, which suggest that the growth of NPF-originated particles accounted up to ∼60% of the accumulation mode particles in the Beijing–Tianjin–Hebei area during haze conditions. The results suggest that a reduction in anthropogenic gaseous precursors, suppressing particle growth, is a critical step for alleviating haze although the number concentration of freshly formed particles (3–40 nm) via NPF does not reduce after emission controls.


The Holocene ◽  
2021 ◽  
pp. 095968362110032
Author(s):  
Pingyuan Li ◽  
Mingkun Li ◽  
Huayang Gan ◽  
Zhen Xia

Typhoon is an important meteorological phenomenon that affects the living and development of human beings on the southern China coast. However, there is still lack of clarity in the paleo-typhoon history and its influence on the evolution of the ancient human settlement environment since the mid-Holocene. Here, we identify six typhoon-like deposits from a core retrieved from the northern South China Sea shelf, close to the Pearl River Estuary, based on accelerated mass spectrometry 14C dating, grain size, and geochemistry. The sand fractions, CaO, Sr, SiO2/TiO2, and SiO2/Al2O3 were used to indicate the typhoon-like deposits. Results show that the ages with high-frequency typhoons are present ~200–300 cal yr BP, ~800–1000 cal yr BP, ~1500–1700 cal yr BP, ~2000–2100 cal yr BP, ~2400–2500 cal yr BP, and ~2700–3000 cal yr BP. Our results are comparable to the records from adjacent regions. Significantly, the vast tides occurred in the duration of ~2700–3000 cal yr BP in southern China, which probably caused the ancestors’ migration to the inland. Further studies are needed to deeply study the paleo-typhoon history in the southern China coast to verify our results.


2012 ◽  
Vol 12 (3) ◽  
pp. 1497-1513 ◽  
Author(s):  
X. Li ◽  
T. Brauers ◽  
R. Häseler ◽  
B. Bohn ◽  
H. Fuchs ◽  
...  

Abstract. We performed measurements of nitrous acid (HONO) during the PRIDE-PRD2006 campaign in the Pearl River Delta region 60 km north of Guangzhou, China, for 4 weeks in June 2006. HONO was measured by a LOPAP in-situ instrument which was setup in one of the campaign supersites along with a variety of instruments measuring hydroxyl radicals, trace gases, aerosols, and meteorological parameters. Maximum diurnal HONO mixing ratios of 1–5 ppb were observed during the nights. We found that the nighttime build-up of HONO can be attributed to the heterogeneous NO2 to HONO conversion on ground surfaces and the OH + NO reaction. In addition to elevated nighttime mixing ratios, measured noontime values of ≈200 ppt indicate the existence of a daytime source higher than the OH + NO→HONO reaction. Using the simultaneously recorded OH, NO, and HONO photolysis frequency, a daytime additional source strength of HONO (PM) was calculated to be 0.77 ppb h−1 on average. This value compares well to previous measurements in other environments. Our analysis of PM provides evidence that the photolysis of HNO3 adsorbed on ground surfaces contributes to the HONO formation.


The Holocene ◽  
2011 ◽  
Vol 22 (6) ◽  
pp. 705-715 ◽  
Author(s):  
Fengling Yu ◽  
Yongqiang Zong ◽  
Jeremy M Lloyd ◽  
Melanie J Leng ◽  
Adam D Switzer ◽  
...  

2018 ◽  
Author(s):  
Hui Yun ◽  
Weihao Wang ◽  
Tao Wang ◽  
Men Xia ◽  
Chuan Yu ◽  
...  

Abstract. Nitrate (NO3−) has become a major component of fine particulate matter (PM2.5) during hazy days in China. However, the role of the heterogeneous reactions of dinitrogen pentoxide (N2O5) in nitrate formation is not well constrained. In January 2017, a severe haze event occurred in the Pearl River Delta (PRD) of southern China during which high levels of PM2.5 (~ 400 μg m−3) and O3 (~ 160 ppbv) were observed at a semi-rural site (Heshan) in the western PRD. Nitrate concentrations were up to 108 μg m−3 (1 h time resolution), and the contribution of nitrate to PM2.5 reached nearly 40 %. Concurrent increases in NO3− and ClNO2 (with a maximum value of 8.3 ppbv in 1 min time resolution) were observed in the first several hours after sunset, indicating an intense N2O5 heterogeneous uptake on aerosols. The formation potential of NO3− via N2O5 heterogeneous reactions was estimated to be 39.7 to 77.3 μg m−3 in the early hours (3 to 6 h) after sunset based on the measurement data, which could completely explain the measured increase in the NO3− concentration during the same time period. Daytime production of nitric acid from the gas-phase reaction of OH + NO2 was calculated with a chemical box model built using the Master Chemical Mechanism (MCM v3.3.1) and constrained by the measurement data. The integrated nocturnal nitrate formed via N2O5 chemistry was comparable to or even higher than the nitric acid formed during the daytime. This study confirms that N2O5 heterogeneous chemistry was a significant source of aerosol nitrate during hazy days in southern China.


Author(s):  
Xiangbo Feng ◽  
Wei Zhang ◽  
Zhenglei Zhu ◽  
Amulya Chevuturi ◽  
Wenlong Chen

AbstractUnderstanding water level (WL) fluctuations in river deltas is of importance for managing water resources and minimizing the impacts of floods and droughts. Here, we demonstrate the competing effects of atmospheric and oceanic forcing on multi-timescale variability and changes in the Pearl River Delta (PRD) WLs in southern China, using 52 years (1961–2012) of in-situ observations at 13 hydrological stations. PRD WL presents significant seasonal to decadal variations, with large amplitudes upstream related to strong variability of southern China rainfall, and with relatively small amplitudes at the coastal stations determined by sea level (SL) fluctuations of the northern South China Sea. We find that the strengths of atmospheric and oceanic forcing in PRD are not mutually independent, leading to a distinct contrast of WL–forcing relationships at upstream and coastal stations. In the transition zone, because of counteracts of atmospheric and oceanic forcing, no robust relationships are identified between WL and either of the forcing. We further show that in the drought season of the warm ENSO and PDO epochs, the effect of atmospheric (oceanic) forcing on PRD WL is largely enhanced (weakened), due to increased southern China rainfall and negative SL anomalies. Over the observation period, WL significantly decreased at upstream stations, by up to 28–42 mm/year for flood season, contrasting with the upward trends of <4.3 mm/year at coastal stations across all seasons. Southern China rainfall explains little of the observed WL trends, whilst SL rise is mostly responsible for the WL trends at coastal stations.


2020 ◽  
Vol 20 (19) ◽  
pp. 11451-11467
Author(s):  
Zhenhao Ling ◽  
Qianqian Xie ◽  
Min Shao ◽  
Zhe Wang ◽  
Tao Wang ◽  
...  

Abstract. The dicarbonyls glyoxal (Gly) and methylglyoxal (Mgly) have been recognized as important precursors of secondary organic aerosols (SOAs) through the atmospheric heterogeneous process. In this study, field measurement was conducted at a receptor site in the Pearl River Delta (PRD) region in southern China, and an observation-based photochemical box model was subsequently applied to investigate the production and evolution of Gly and Mgly as well as their contributions to SOA formation. The model was coupled with a detailed gas-phase oxidation mechanism of volatile organic compounds (VOCs) (i.e., Master Chemical Mechanism, MCM, v3.2), heterogeneous processes of Gly and Mgly (i.e., reversible partitioning in aqueous phase, irreversible volume reactions and irreversible surface uptake processes), and the gas–particle partitioning of oxidation products. The results suggested that without considering the heterogeneous processes of Gly and Mgly on aerosol surfaces, the model would overpredict the mixing ratios of Gly and Mgly by factors of 3.3 and 3.5 compared to the observed levels. The agreement between observation and simulation improved significantly when the irreversible uptake and the reversible partitioning were incorporated into the model, which in total both contributed ∼ 62 % to the destruction of Gly and Mgly during daytime. Further analysis of the photochemical budget of Gly and Mgly showed that the oxidation of aromatics by the OH radical was the major pathway producing Gly and Mgly, followed by degradation of alkynes and alkenes. Furthermore, based on the improved model mechanism, the contributions of VOC oxidation to SOA formed from gas–particle partitioning (SOAgp) and from heterogeneous processes of Gly and Mgly (SOAhet) were also quantified. It was found that o-xylene was the most significant contributor to SOAgp formation (∼ 29 %), while m,p-xylene and toluene made dominant contributions to SOAhet formation. Overall, the heterogeneous processes of Gly and Mgly can explain ∼ 21 % of SOA mass in the PRD region. The results of this study demonstrated the important roles of heterogeneous processes of Gly and Mgly in SOA formation and highlighted the need for a better understanding of the evolution of intermediate oxidation products.


Sign in / Sign up

Export Citation Format

Share Document