7 research outputs found
Narrowing Differences in Urban and Nonurban Surface Ozone in the Northern Hemisphere Over 1990–2020
Surface ozone air pollution is unequally distributed
in space and
varies over urban and surrounding nonurban areas. Traditionally, urban
ozone levels tend to be lower than their nonurban counterparts, resulting
from discrepancies in emissions and nonlinearity in photochemistry.
However, how the differences in urban vs nonurban ozone evolve over
the past decades is uncertain. Here, we construct 6361 pairs of urban
and nonurban ozone measurement sites based on available surface monitoring
networks to analyze the long-term changes of their ozone differences.
We show that urban vs nonurban ozone differences have narrowed substantially
in North America, Europe, South Korea, and Japan over the summers
of 1990–2020. The hemispheric mean urban vs nonurban ozone
differences have decreased by 90% from −5.0 ppbv in the 1990s
to −0.5 ppbv in the 2010s. We estimate that the anthropogenic
emission reduction of nitrogen oxides is the dominant driver of the
narrowing trends. It has suppressed the urban ozone titration and
led to closer ozone formation regimes over urban and nonurban areas
Base-Promoted Tandem Synthesis of 2‑Substituted Indoles and <i>N</i>‑Fused Polycyclic Indoles
Herein is developed a base-promoted approach for the
synthesis
of C2-substituted indoles and N-fused polycyclic
indoles via 5-endo-dig cyclization
of 2-alkynyl anilines, followed by a 1,3′-acyl migration or
a dearomatizing Michael addition process. A range of N–H free
indoles and 8,9-dihydropyrido[1,2-a]indol-6(7H)-one scaffolds were synthesized in good to excellent yields
with broad scope
Severe Surface Ozone Pollution in China: A Global Perspective
The nationwide extent
of surface ozone pollution in China and its
comparison to the global ozone distribution have not been recognized
because of the scarcity of Chinese monitoring sites before 2012. Here
we address this issue by using the latest 5 year (2013–2017)
surface ozone measurements from the Chinese monitoring network, combined
with the recent Tropospheric Ozone Assessment Report (TOAR) database
for other industrialized regions such as Japan, South Korea, Europe,
and the United States (JKEU). We use various human health and vegetation
exposure metrics. We find that although the median ozone values are
comparable between Chinese and JKEU cities, the magnitude and frequency
of high-ozone events are much larger in China. The national warm-season
(April–September) fourth highest daily maximum 8 h average
(4MDA8) ozone level (86.0 ppb) and the number of days with MDA8 values
of >70 ppb (NDGT70, 29.7 days) in China are 6.3–30% (range
of regional mean differences) and 93–575% higher, respectively,
than the JKEU regional averages. Health exposure metrics such as warm-season
mean MDA8 and annual SOMO35 (sum of ozone means over 35 ppb) are 6.3–16
and 25–95% higher in China, respectively. We also find an increase
in the surface ozone level over China in 2016 and 2017 relative to
2013 and 2014. Our results show that on the regional scale the exposure
of humans and vegetation to ozone is greater in China than in other
developed regions of the world with comprehensive ozone monitoring
Aerosol Liquid Water Driven by Anthropogenic Inorganic Salts: Implying Its Key Role in Haze Formation over the North China Plain
This study reveals aerosol liquid
water content (ALWC) in PM<sub>2.5</sub> ranged from 2% up to 74%,
and the associated secondary
inorganic fraction rose from 24% to 55%, while ambient relative humidity
(RH) increased from 15% to 83% in the atmosphere over Beijing. Unexpectedly,
the secondary inorganic fraction in PM<sub>2.5</sub> increased with
an increase in the ambient RH, which is a meteorological parameter
independent of anthropogenic activities, indicating the presence of
a feedback mechanism driven by Henry’s law and thermodynamic
equilibrium. During haze episodes, simultaneously elevated RH levels
and anthropogenic secondary inorganic mass concentrations resulted
in an abundant ALWC. The condensed water could act as an efficient
medium for multiphase reactions, thereby facilitating the transformation
of reactive gaseous pollutants into particles and accelerating the
formation of heavy haze. ALWC was well correlated with the mass concentrations
of both nitrate and sulfate, indicating both nitrate and sulfate salts
play key roles in determining ALWC. Coincident with a significant
reduction in SO<sub>2</sub> emissions throughout China, nitrates will
become a dominant anthropogenic inorganic salt driving ALWC. Thus,
the abundance of ALWC and its effects on the aerosol chemistry and
climate should be reconsidered
Multiple Impacts of Aerosols on O<sub>3</sub> Production Are Largely Compensated: A Case Study Shenzhen, China
Tropospheric ozone (O3) is a harmful gas compound
to
humans and vegetation, and it also serves as a climate change forcer.
O3 is formed in the reactions of nitrogen oxides and volatile
organic compounds (VOCs) with light. In this study, an O3 pollution episode encountered in Shenzhen, South China in 2018 was
investigated to illustrate the influence of aerosols on local O3 production. We used a box model with comprehensive heterogeneous
mechanisms and empirical prediction of photolysis rates to reproduce
the O3 episode. Results demonstrate that the aerosol light
extinction and NO2 heterogeneous reactions showed comparable
influence but opposite signs on the O3 production. Hence,
the influence of aerosols from different processes is largely counteracted.
Sensitivity tests suggest that O3 production increases
with further reduction in aerosols in this study, while the continued
NOx reduction finally shifts O3 production to an NOx-limited regime
with respect to traditional O3–NOx-VOC sensitivity. Our results shed light on the role of NOx reduction on O3 production and
highlight further mitigation in NOx not
only limiting the production of O3 but also helping to
ease particulate nitrate, as a path for cocontrol of O3 and fine particle pollution
High N<sub>2</sub>O<sub>5</sub> Concentrations Observed in Urban Beijing: Implications of a Large Nitrate Formation Pathway
The
heterogeneous hydrolysis of dinitrogen pentoxide (N<sub>2</sub>O<sub>5</sub>) is important to understanding the formation of particulate
nitrate (pNO<sub>3</sub><sup>–</sup>). Measurements of N<sub>2</sub>O<sub>5</sub> in the surface layer taken at an urban site
in Beijing are presented here. N<sub>2</sub>O<sub>5</sub> was observed
with large day-to-day variability. High N<sub>2</sub>O<sub>5</sub> concentrations were determined during pollution episodes with the
co-presence of large aerosol loads. The maximum value was 1.3 ppbv
(5 s average), associated with an air mass characterized by a high
level of O<sub>3</sub>. N<sub>2</sub>O<sub>5</sub> uptake coefficients
were estimated to be in the range of 0.025–0.072 using the
steady-state lifetime method. As a consequence, the nocturnal pNO<sub>3</sub><sup>–</sup> formation potential by N<sub>2</sub>O<sub>5</sub> heterogeneous uptake was calculated to be 24–85 μg
m<sup>–3</sup> per night and, on average, 57 μg m<sup>–3</sup> during days with pollution. This was comparable to
or even higher than that formed by the partitioning of HNO<sub>3</sub>. The results highlight that N<sub>2</sub>O<sub>5</sub> heterogeneous
hydrolysis is vital in pNO<sub>3</sub><sup>–</sup> formation
in Beijing