Investigating sulfate formation processes is important not only for air pollution control but also for understanding the climate system. Although the mechanisms of secondary sulfate production have been widely studied, in situ observational evidence implicating an important role of NO₂ in SO₂ oxidation in the real atmosphere has been rare. In this study, we report two unique cases, from an intensive campaign conducted at the Station for Observing Regional Processes of the Earth System (SORPES) in East China, showing distinctly different mechanisms of sulfate formation by NO₂ and related nitrogen chemistry. The first case occurred in an episode of mineral dust mixed with anthropogenic pollutants and especially high concentrations of NO_x. It reveals that NO₂ played an important role, not only in surface catalytic reactions of SO₂ but also in dust‐induced photochemical heterogeneous reactions of NO₂, which produced additional sources of OH radicals to promote new particle formation and growth. The second case was caused by aqueous oxidation of S(IV) by NO₂ under foggy/cloudy conditions with high NH₃ concentration. As a by‐product, the formed nitrite enhanced HONO formation and further promoted the gas‐phase formation of sulfate in the downwind area. This study highlights the effect of NO_x in enhancing the atmospheric oxidizing capacity and indicates a potentially very important impact of increasing NO_x on particulate pollution formation and regional climate change in East Asia.

The western Pacific subtropical high (WPSH) is regarded as the key circulation system that dominates the summer heat waves over eastern China, but whether the WPSH–summer heat wave connection changes with time remains unknown. In this study, decadal variations in the WPSH–heat wave connection were examined for the period 1959–2016 using daily maximum temperature data from 654 observational stations across China and global reanalysis datasets. The results show that the correlation coefficient between the WPSH intensity (WPSHI) and the number of heat-wave days (NHD) was 0.65 (>99% confidence level) during positive phases of the Pacific decadal oscillation (PDO), whereas that during negative phases of the PDO was only 0.12 (<80% confidence level). The remarkable difference in correlations is due to the more westward extension of a stronger WPSH in El Niño decaying summers during the positive phases of PDO. The stronger Indian Ocean warming in El Niño decaying-year summers for PDO positive phases in comparison to PDO negative phases is associated with enhanced convection and heating, which further drive a stronger anticyclone over the northwestern Pacific, leading to a stronger and more westward-extending WPSH, which is favorable for more heat waves over eastern China.

Atmospheric mercury (Hg) is a global pollutant and thought to be the main source of mercury in oceanic and remote terrestrial systems, where it becomes methylated and bioavailable; hence, atmospheric mercury pollution has global consequences for both human and ecosystem health. Understanding of spatial and temporal variations of atmospheric speciated mercury can advance our knowledge of mercury cycling in various environments. This review summarized spatiotemporal variations of total gaseous mercury or gaseous elemental mercury (TGM/GEM), gaseous oxidized mercury (GOM), and particulate-bound mercury (PBM) in various environments including oceans, continents, high elevation, the free troposphere, and low to high latitudes. In the marine boundary layer (MBL), the oxidation of GEM was generally thought to drive the diurnal and seasonal variations of TGM/GEM and GOM in most oceanic regions, leading to lower GEM and higher GOM from noon to afternoon and higher GEM during winter and higher GOM during spring–summer. At continental sites, the driving mechanisms of TGM/GEM diurnal patterns included surface and local emissions, boundary layer dynamics, GEM oxidation, and for high-elevation sites mountain–valley winds, while oxidation of GEM and entrainment of free tropospheric air appeared to control the diurnal patterns of GOM. No pronounced diurnal variation was found for Tekran measured PBM at MBL and continental sites. Seasonal variations in TGM/GEM at continental sites were attributed to increased winter combustion and summertime surface emissions, and monsoons in Asia, while those in GOM were controlled by GEM oxidation, free tropospheric transport, anthropogenic emissions, and wet deposition. Increased PBM at continental sites during winter was primarily due to local/regional coal and wood combustion emissions. Long-term TGM measurements from the MBL and continental sites indicated an overall declining trend. Limited measurements suggested TGM/GEM increasing from the Southern Hemisphere (SH) to the Northern Hemisphere (NH) due largely to the vast majority of mercury emissions in the NH, and the latitudinal gradient was insignificant in summer probably as a result of stronger meridional mixing. Aircraft measurements showed no significant vertical variation in GEM over the field campaign regions; however, depletion of GEM was observed in stratospherically influenced air masses. In examining the remaining questions and issues, recommendations for future research needs were provided, and among them is the most imminent need for GOM speciation measurements and fundamental understanding of multiphase redox kinetics.