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Sulfur dioxide and nitrogen oxide emissions from shipping have been regulated internationally for more than fifteen years. Emissions reduction from shipping provides benefits for human health and the environment, but the effectiveness of regulations in reducing ship emissions is less well understood. Here, we examine how the establishment of European Emission Control Areas and other international maritime regulations in the North and Baltic Seas affect sulfur dioxide and nitrogen oxide emissions in the region. We combine and analyze more than 110,000 ship plume measurements, inspection results, and satellite data from 2018 to 2022. We find that compliance rates for sulfur emissions are higher near ports than in open waters. However, the regulations did not affect the concentration of nitrogen oxide emissions, which increased in the past three years. These findings highlight the need for enhanced emission regulations that improve air quality.

International shipping’s particulate matter primary emissions have a share in global anthropogenic emissions of between 3% and 4%. Ship emissions of volatile organic compounds (VOCs) can play an important role in the formation of fine particulate matter. Using an aerosol box model for the near-plume scale, this study investigated how the changing VOC emission factor (EF) for ship engines impacts the formation of secondary PM2.5 in ship exhaust plumes that were detected during a measurement campaign. The agreement between measured and modeled particle number size distribution was improved by adjusting VOC emissions, in particular of intermediate-, low-, and extremely low-volatility compounds. The scaling of the VOC emission factor showed that the initial emission factor, based on literature data, had to be multiplied by 3.6 for all VOCs. Information obtained from the box model was integrated into a regional-scale chemistry transport model (CTM) to study the influence of changed VOC ship emissions over the Mediterranean Sea. The regional-scale CTM run with adjusted ship emissions indicated a change in PM2.5 of up to 5% at the main shipping routes and harbor cities in summer. Nevertheless, overall changes due to a change in the VOC EF were rather small, indicating that the size of grid cells in CTMs leads to a fast dilution.

Goal of the project CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrumented Container) is to carry out regular and detailed observations of atmospheric composition (particles and gases) at cruising altitudes of passenger aircraft, i.e. at 9–12 km. Mercury has been measured since May 2005 by a modified Tekran instrument (Tekran Model 2537 A analyser, Tekran Inc., Toronto, Canada) during monthly intercontinental flights between Europe and South and North America, Africa, and Asia. Here we describe the instrument modifications, the post-flight processing of the raw instrument signal, and the fractionation experiments.

Tropospheric sections of flights with the CARIBIC (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrumented Container) observatory from May 2005 until June 2013, are investigated for the occurrence of plumes with elevated Hg concentrations. Additional information on CO, CO2, CH4, NOy, O3, hydrocarbons, halocarbons, acetone and acetonitrile enable us to attribute the plumes to biomass burning, urban/industrial sources or a mixture of both. Altogether, 98 pollution plumes with elevated Hg concentrations and CO mixing ratios were encountered, and the Hg/CO emission ratios for 49 of them could be calculated. Most of the plumes were found over East Asia, in the African equatorial region, over South America and over Pakistan and India. The plumes encountered over equatorial Africa and over South America originate predominantly from biomass burning, as evidenced by the low Hg/CO emission ratios and elevated mixing ratios of acetonitrile, CH3Cl and particle concentrations. The backward trajectories point to the regions around the Rift Valley and the Amazon Basin, with its outskirts, as the source areas. The plumes encountered over East Asia and over Pakistan and India are predominantly of urban/industrial origin, sometimes mixed with products of biomass/biofuel burning. Backward trajectories point mostly to source areas in China and northern India. The Hg/CO2 and Hg/CH4 emission ratios for several plumes are also presented and discussed.

Ships are an important source of SO2 and NOx, which are key parameters of air quality. Monitoring of ship emissions is usually carried out using in situ instruments on land, which depend on favourable wind conditions to transport the emitted substances to the measurement site. Remote sensing techniques such as long-path differential optical absorption spectroscopy (LP-DOAS) measurements can supplement those measurements, especially in unfavourable meteorological conditions. In this study 1 year of LP-DOAS measurements made across the river Elbe close to Hamburg (Germany) have been evaluated. Peaks (i.e. elevated concentrations) in the NO2 and SO2 time series were assigned to passing ships, and a method to derive emission rates of SO2, NO2 and NOx from those measurements using a Gaussian plume model is presented. A total of 7402 individual ship passages have been monitored, and their respective NOx, SO2 and NO2 emission rates have been derived. The emission rates, coupled with the knowledge of the ship type, ship size and ship speed, have been analysed. Emission rates are compared to emission factors from previous studies and show good agreement. In contrast to emission factors (in grams per kilogram fuel), the derived emission rates (in grams per second) do not need further knowledge about the fuel consumption of the ship. To our knowledge this is the first time emission rates of air pollutants from individual ships have been derived from LP-DOAS measurements.

The atmospheric deposition of mercury (Hg) occurs via several mechanisms, including dry and wet scavenging by precipitation events. In an effort to understand the atmospheric cycling and seasonal depositional characteristics of Hg, wet deposition samples were collected for approximately 5 years at 17 selected GMOS monitoring sites located in the Northern and Southern hemispheres in the framework of the Global Mercury Observation System (GMOS) project. Total mercury (THg) exhibited annual and seasonal patterns in Hg wet deposition samples. Interannual differences in total wet deposition are mostly linked with precipitation volume, with the greatest deposition flux occurring in the wettest years. This data set provides a new insight into baseline concentrations of THg concentrations in precipitation worldwide, particularly in regions such as the Southern Hemisphere and tropical areas where wet deposition as well as atmospheric Hg species were not investigated before, opening the way for future and additional simultaneous measurements across the GMOS network as well as new findings in future modeling studies.

Long-term measurements of gaseous elemental mercury (GEM) concentrations at Cape Point, South Africa, reveal a downward trend between September 1995 and December 2005 and an upward one from March 2007 until June 2015, implying a change in trend sign between 2004 and 2007. The trend change is qualitatively consistent with the trend changes in GEM concentrations observed at Mace Head, Ireland, and in mercury wet deposition over North America, suggesting a change in worldwide mercury emissions. Seasonally resolved trends suggest a modulation of the overall trend by regional processes. The trends in absolute terms (downward in 1995–2004 and upward in 2007–2015) are highest in austral spring (SON), coinciding with the peak in emissions from biomass burning in South America and southern Africa. The influence of trends in biomass burning is further supported by a biennial variation in GEM concentration found here and an El Niño–Southern Oscillation (ENSO) signature in GEM concentrations reported recently.

The fuel sulfur content (FSC) of ocean-going and inland vessels was measured simultaneously by eight different state-of-the-art and novel monitoring systems during a 6-week campaign at the Elbe River, at a distance of about 10 km to the port of Hamburg, Germany. Both stationary and airborne systems on unoccupied aerial vehicles (UAVs) were operated by four participating partners in a side-by-side measurement setup to measure the emission factors of the same emission sources. A novel laser spectrometer, with significantly better-precision specifications as compared with the other instruments, was used for the first time for emission monitoring regarding the International Convention for the Prevention of Pollution from Ships (MARPOL) Annex VI regulations. The comparison took place in the North Sea sulfur emission control area (SECA), where the allowed FSC is limited to 0.10 %Sm/m. The unit %Sm/m relates to the percentage of mass sulfur per mass combusted fuel. In total, 966 plumes that originated from 436 different vessels were analysed in this study. At the same time, fuel samples obtained from 34 different vessels and bunker delivery notes (BDNs) from five frequently monitored vessels were used as a reference to assess the uncertainties of the different systems. Seven of the eight measurement systems tended to underestimate the FSC found from fuel samples and BDNs. A possible relation between underestimation and high relative humidities (above 80 %) was observed. The lowest systematic deviations were observed for the airborne systems and the novel laser spectrometer. The two UAV-borne systems showed total uncertainties of 0.07 %Sm/m and 0.09 %Sm/m (confidence level: 95 %). The novel laser spectrometer showed the lowest total uncertainty of 0.05 %Sm/m compared with other stationary sniffer systems, whose total uncertainties range from 0.08 %Sm/m to 0.09 %Sm/m. It was concluded that non-compliant vessels, with an actual FSC of the combusted fuel above 0.15 %Sm/m to 0.19 %Sm/m, can be detected by the compared systems with 95 % confidence.

Mercury was measured onboard the IAGOS-CARIBIC passenger aircraft from May 2005 until February 2016 during near monthly sequences of mostly four intercontinental flights from Germany to destinations in North and South America, Africa and South and East Asia. Most of these mercury data were obtained using an internal default signal integration procedure of the Tekran instrument but since April 2014 more precise and accurate data were obtained using post-flight manual integration of the instrument raw signal. In this paper we use the latter data.Increased upper tropospheric total mercury (TM) concentrations due to large scale biomass burning were observed in the upper troposphere (UT) at the equator and southern latitudes during the flights to Latin America and South Africa in boreal autumn (SON) and boreal winter (DJF). TM concentrations in the lowermost stratosphere (LMS) decrease with altitude above the thermal tropopause but the gradient is less steep than reported before. Seasonal variation of the vertical TM distribution in the UT and LMS is similar to that of other trace gases with surface sources and stratospheric sinks. Speciation experiments suggest comparable TM and gaseous elementary mercury (GEM) concentrations at and below the tropopause leaving little space for Hg2+ (TM − GEM) being the dominating component of TM here. In the stratosphere significant GEM concentrations were found to exist up to 4 km altitude above the thermal tropopause. Correlations with N2O as a reference tracer suggest stratospheric lifetimes of 72±37 and 74±27 years for TM and GEM, respectively, comparable to the stratospheric lifetime of COS. This coincidence, combined with pieces of evidence from us and other researchers, corroborates the hypothesis that Hg2+ formed by oxidation in the stratosphere attaches to sulfate particles formed mainly by oxidation of COS and is removed with them from the stratosphere by air mass exchange, gravitational sedimentation and cloud scavenging processes.

Atmospheric chemistry and transport of mercury play a key role in the global mercury cycle. However, there are still considerable knowledge gaps concerning the fate of mercury in the atmosphere. This is the second part of a model intercomparison study investigating the impact of atmospheric chemistry and emissions on mercury in the atmosphere. While the first study focused on ground-based observations of mercury concentration and deposition, here we investigate the vertical and interhemispheric distribution and speciation of mercury from the planetary boundary layer to the lower stratosphere. So far, there have been few model studies investigating the vertical distribution of mercury, mostly focusing on single aircraft campaigns. Here, we present a first comprehensive analysis based on various aircraft observations in Europe, North America, and on intercontinental flights. The investigated models proved to be able to reproduce the distribution of total and elemental mercury concentrations in the troposphere including interhemispheric trends. One key aspect of the study is the investigation of mercury oxidation in the troposphere. We found that different chemistry schemes were better at reproducing observed oxidized mercury patterns depending on altitude. High concentrations of oxidized mercury in the upper troposphere could be reproduced with oxidation by bromine while elevated concentrations in the lower troposphere were better reproduced by OH and ozone chemistry. However, the results were not always conclusive as the physical and chemical parameterizations in the chemistry transport models also proved to have a substantial impact on model results.