ALBERT

Description: The number of vehicles in China has been increasing rapidly. We evaluate the impact of current and possible future vehicle emissions from China on Asian air quality. We modify the Regional Emission Inventory in Asia (REAS) for China's road transport sector in 2000 using updated Chinese data for the number of vehicles, annual mileage, and emission factors. We develop two scenarios for 2020: a scenario where emission factors remain the same as they were in 2000 (No-Policy, NoPol), and a scenario where Euro 3 vehicle emission standards are applied to all vehicles (except motorcycles and rural vehicles). The Euro 3 scenario is an approximation of what may be the case in 2020 as, starting in 2008, all new vehicles in China (except motorcycles) were required to meet the Euro 3 emission standards. Using the Weather Research and Forecasting model coupled with Chemistry (WRF/Chem), we examine the regional air quality response to China's vehicle emissions in 2000 and in 2020 for the NoPol and Euro 3 scenarios. We evaluate the 2000 model results with observations in Japan, China, Korea, and Russia. Under NoPol in 2020, emissions of carbon monoxide (CO), nitrogen oxides (NOx), non-methane volatile organic compounds (NMVOCs), black carbon (BC), and organic carbon (OC) from China's vehicles more than double compared to the 2000 baseline. If all vehicles meet the Euro 3 regulations in 2020, however, these emissions are reduced by more than 50% relative to NoPol. The implementation of stringent vehicle emission standards leads to a large, simultaneous reduction of the surface ozone (O3) mixing ratios and particulate matter (PM2.5) concentrations. In the Euro 3 scenario, surface O3 is reduced by more than 10 ppbv and surface PM2.5 is reduced by more than 10 μg m−3 relative to NoPol in Northeast China in all seasons. In spring, surface O3 mixing ratios and PM2.5 concentrations in neighboring countries are also reduced by more than 3 ppbv and 1 μg m−3, respectively. We find that effective regulation of China's road transport sector will be of significant benefit for air quality both within China and across East Asia as well.

Description: HCFC-22 (CHClF2, chlorodifluoromethane) is an ozone-depleting substance (ODS) as well as a significant greenhouse gas (GHG). HCFC-22 has been used widely as a refrigerant fluid in cooling and air-conditioning equipment since the 1960s, and it has also served as a traditional substitute for some chlorofluorocarbons (CFCs) controlled under the Montreal Protocol. A low frequency record on tropospheric HCFC-22 since the late 1970s is available from measurements of the Southern Hemisphere Cape Grim Air Archive (CGAA) and a few Northern Hemisphere air samples (mostly from Trinidad Head) using the Advanced Global Atmospheric Gases Experiment (AGAGE) instrumentation and calibrations. Since the 1990s high-frequency, high-precision, in situ HCFC-22 measurements have been collected at these AGAGE stations. Since 1992, the Global Monitoring Division of the National Oceanic and Atmospheric Administration/Earth System Research Laboratory (NOAA/ESRL) has also collected flasks on a weekly basis from remote sites across the globe and analyzed them for a suite of halocarbons including HCFC-22. Additionally, since 2006 flasks have been collected approximately daily at a number of tower sites across the US and analyzed for halocarbons and other gases at NOAA. All results show an increase in the atmospheric mole fractions of HCFC-22, and recent data show a growth rate of approximately 4% per year, resulting in an increase in the background atmospheric mole fraction by a factor of 1.7 from 1995 to 2009. Using data on HCFC-22 consumption submitted to the United Nations Environment Programme (UNEP), as well as existing bottom-up emission estimates, we first create globally-gridded a priori HCFC-22 emissions over the 15 yr since 1995. We then use the three-dimensional chemical transport model, Model for Ozone and Related Chemical Tracers version 4 (MOZART v4), and a Bayesian inverse method to estimate global as well as regional annual emissions. Our inversion indicates that the global HCFC-22 emissions have an increasing trend between 1995 and 2009. We further find a surge in HCFC-22 emissions between 2005 and 2009 from developing countries in Asia – the largest emitting region including China and India. Globally, substantial emissions continue despite production and consumption being phased out in developed countries currently.

Description: HCFC-22 (CHClF_2, chlorodifluoromethane) is an ozone-depleting substance (ODS) as well as a significant greenhouse gas (GHG). HCFC-22 has been used widely as a refrigerant fluid in cooling and air-conditioning equipment since the 1960s, and it has also served as a traditional substitute for some chlorofluorocarbons (CFCs) controlled under the Montreal Protocol. A low frequency record on tropospheric HCFC-22 since the late 1970s is available from measurements of the Southern Hemisphere Cape Grim Air Archive (CGAA) and a few Northern Hemisphere air samples (mostly from Trinidad Head) using the Advanced Global Atmospheric Gases Experiment (AGAGE) instrumentation and calibrations. Since the 1990s high-frequency, high-precision, in situ HCFC-22 measurements have been collected at these AGAGE stations. Since 1992, the Global Monitoring Division of the National Oceanic and Atmospheric Administration/Earth System Research Laboratory (NOAA/ESRL) has also collected flasks on a weekly basis from remote sites across the globe and analyzed them for a suite of halocarbons including HCFC-22. Additionally, since 2006 flasks have been collected approximately daily at a number of tower sites across the US and analyzed for halocarbons and other gases at NOAA. All results show an increase in the atmospheric mole fractions of HCFC-22, and recent data show a growth rate of approximately 4% per year, resulting in an increase in the background atmospheric mole fraction by a factor of 1.7 from 1995 to 2009. Using data on HCFC-22 consumption submitted to the United Nations Environment Programme (UNEP), as well as an existing bottom-up emissions estimate, we first create globally-gridded a priori HCFC-22 emissions over the 15 yr since 1995. We then use the three-dimensional chemical transport model, Model for Ozone and Related Chemical Tracers version 4 (MOZART v4) and a Bayesian inverse method to estimate global as well as regional annual emissions. Our inversion indicates that the global HCFC-22 emissions have an increasing trend between 1995 and 2009. We further find a surge in HCFC-22 emissions in 2009 from developing countries in Asia – the largest emitting region including China and India. Globally, substantial emissions continue despite current phase-out of production and consumption in developed countries.

Description: The number of vehicles in China has been increasing rapidly. We evaluate the impact of current and possible future vehicle emissions from China on Asian air quality. We modify the Regional Emission Inventory in Asia (REAS) for China's road transport sector in 2000 using updated Chinese data for vehicle numbers, annual mileage and emission factors. We develop two scenarios for 2020: a scenario where emission factors remain the same as they were before any regulation was implemented (business-as-usual, BAU), and a scenario where Euro 3 vehicle emission standards are applied to all vehicles (except motorcycles and rural vehicles). The Euro 3 scenario is an approximation of what may be the case in 2020 as, starting in 2008, all new gasoline and diesel vehicles in China (except motorcycles) were required to meet the Euro 3 emission standards. Using the Weather Research and Forecasting model coupled with Chemistry (WRF/Chem), we examine the regional air quality response to China's vehicle emissions in 2000 and in 2020 for the BAU and Euro 3 scenarios. We evaluate the 2000 model results with observations in Japan, China, Korea, and Russia. Under BAU in 2020, emissions of carbon monoxide (CO), nitrogen oxides (NOx), non-methane volatile organic compounds (NMVOCs), black carbon (BC) and organic carbon (OC) from China's vehicles more than double compared to the 2000 baseline. If all vehicles meet the Euro 3 regulations in 2020, however, these emissions are reduced by more than 50% relative to BAU. The implementation of stringent vehicle emission standards leads to a large, simultaneous reduction of the surface ozone (O3) mixing ratios and particulate matter (PM2.5) concentrations. In the Euro 3 scenario, surface O3 is reduced by more than 10 ppbv and surface PM2.5 is reduced by more than 10 μg m−3 relative to BAU in Northeast China in all seasons. In spring, surface O3 mixing ratios and PM2.5 concentrations in neighboring countries are also reduced by more than 3 ppbv and 1 μg m−3, respectively. We find that effective regulation of China's road transport sector will be of significant benefit for air quality both within China and across East Asia as well.

Description: The first concerted multi-model intercomparison of halogenated very short-lived substances (VSLS) has been performed, within the framework of the ongoing Atmospheric Tracer Transport Model Intercomparison Project (TransCom). Eleven global models or model variants participated, simulating the major natural bromine VSLS, bromoform (CHBr3) and dibromomethane (CH2Br2), over a 20-year period (1993-2012). The overarching goal of TransCom-VSLS was to provide a reconciled model estimate of the stratospheric source gas injection (SGI) of bromine from these gases, to constrain the current measurement-derived range, and to investigate inter-model differences due to emissions and transport processes.Models ran with standardised idealised chemistry, to isolate differences due to transport, and we investigated the sensitivity of results to a range of VSLS emission inventories. Models were tested in their ability to reproduce the observed seasonal and spatial distribution of VSLS at the surface, using measurements from NOAA’s long-term global monitoring network, and in the tropical troposphere, using recent aircraft measurements - including high altitude observations from the NASA Global Hawk platform. The models generally capture the seasonal cycle of surface CHBr3 and CH2Br2 well, with a strong model-measurement correlation (r ≥ 0.7) and a low sensitivity to the choice of emission inventory, at most sites. In a given model, the absolute model-measurement agreement is highly sensitive to the choice of emissions and inter-model differences are also apparent, even when using the same inventory, highlighting the challenges faced in evaluating such inventories at the global scale. Across the ensemble, most consistency is found within the tropics where most of the models (8 out of 11) achieve optimal agreement to surface CHBr3 observations using the lowest of the three CHBr3 emission inventories tested (similarly, 8 out of 11 models for CH2 Br2). In general, the models are able to reproduce well observations of CHBr3 and CH2 Br2 obtained in the tropical tropopause layer (TTL) at various locations throughout the Pacific. Zonal variability in VSLS loading in the TTL is generally consistent among models, with CHBr3 (and to a lesser extent CH2 Br2) most elevated over the tropical West Pacific during boreal winter. The models also indicate the Asian Monsoon during boreal summer to be an important pathway for VSLS reaching the stratosphere, though the strength of this signal varies considerably among models. We derive an ensemble climatological mean estimate of the stratospheric bromine SGI from CHBr3 and CH2 Br2 of 2.0 (1.2-2.5) ppt, ≫ 57% larger than the best estimate from the most recent World Meteorological Organization (WMO) Ozone Assessment Report. We find no evidence for a long-term, transport-driven trend in the stratospheric SGI of bromine over the simulation period. However, transport-driven inter-annual variability in the annual mean bromine SGI is of the order of a ±5%, with SGI exhibiting a strong positive correlation with ENSO in the East Pacific.

Description: We present a comprehensive estimate of nitrous oxide ( N2O) emissions using observations and models from 1995 to 2008. High-frequency records of tropospheric N2O are available from measurements at Cape Grim, Tasmania; Cape Matatula, American Samoa; Ragged Point, Barbados; Mace Head, Ireland; and at Trinidad Head, California using the Advanced Global Atmospheric Gases Experiment (AGAGE) instrumentation and calibrations. The Global Monitoring Division of the National Oceanic and Atmospheric Administration/Earth System Research Laboratory (NOAA/ESRL) has also discrete air samples collected in flasks and in situ measurements from remote sites across the globe and analyzed them for a suite of species including N2O. In addition to these major networks, we include in situ and aircraft measurements from the National Institute for Environmental Studies (NIES) and flask measurements from the Tohoku University and Commonwealth Scientific and Industrial Research Organization (CSIRO) networks. All measurements show increasing atmospheric mole fractions of N2O, with a varying growth rate of 0.1–0.7 % yr-1, resulting in a 7.4% increase in the background atmospheric mole fraction between 1979 and 2011. Using existing emission inventories as well as bottom-up process modeling results, we first create globally-gridded a priori N2O emissions over the 37 yr since 1975. We then use the three-dimensional chemical transport model, Model for Ozone and Related Chemical Tracers version 4 (MOZART v4), and a Bayesian inverse method to estimate global as well as regional annual emissions for five source sectors from 13 regions in the world. This is the first time that all of these measurements from multiple networks have been combined to determine emissions. Our inversion indicates that global and regional N2O emissions have an increasing trend between 1995 and 2008. Despite large uncertainties, a significant increase is seen from the Asian agricultural sector in the recent years, most likely due to an increase in the use of nitrogenous fertilizers, as has been suggested by previous studies, and also in Asian natural soil.

Description: We present a comparison of chemistry-transport models (TransCom-N2O) to examine the importance of atmospheric transport and surface fluxes on the variability of N2O mixing ratios in the troposphere. Six different models and two model variants participated in the inter-comparison and simulations were made for the period 2006 to 2009. In addition to N2O, simulations of CFC-12 and SF6 were made by a subset of four of the models to provide information on the models proficiency in stratosphere-troposphere exchange (STE) and meridional transport, respectively. The same prior emissions were used by all models to restrict differences among models to transport and chemistry alone. Four different N2O flux scenarios totalling between 14 and 17 Tg N yr−1 (for 2005) globally were also compared. The modelled N2O mixing ratios were assessed against observations from in-situ stations, discrete air sampling networks, and aircraft. All models adequately captured the large-scale patterns of N2O and the vertical gradient from the troposphere to the stratosphere and most models also adequately captured the N2O tropospheric growth rate. However, all models underestimated the inter-hemispheric N2O gradient by at least 0.33 ppb (equivalent to 1.5 Tg N), which, even after accounting for an overestimate of emissions in the Southern Ocean of circa 1.0 Tg N, points to a likely underestimate of the Northern Hemisphere source by up to 0.5 Tg N and/or an overestimate of STE in the Northern Hemisphere. Comparison with aircraft data reveal that the models overestimate the amplitude of the N2O seasonal cycle at Hawaii (21° N, 158° W) below circa 6000 m, suggesting an overestimate of the importance of stratosphere to troposphere transport in the lower troposphere at this latitude. In the Northern Hemisphere, most of the models that provided CFC-12 simulations captured the phase of the CFC-12, seasonal cycle, indicating a reasonable representation of the timing of STE. However, for N2O all models simulated a too early minimum by 2 to 3 months owing to errors in the seasonal cycle in the prior soil emissions, which is still not adequately represented by terrestrial biosphere models. In the Southern Hemisphere, most models failed to capture the N2O and CFC-12 seasonality at Cape Grim, Tasmania, and all failed at the South Pole, whereas for SF6, all models could capture the seasonality at all sites, suggesting that there are large errors in modeled vertical transport in high southern latitudes.

Description: This study examines N2O emission estimates from 5 different atmospheric inversion frameworks. The 5 frameworks differ in the choice of atmospheric transport model, meteorological data, prior uncertainties and inversion method but use the same prior emissions and observation dataset. The mean emissions for 2006 to 2008 are compared in terms of the spatial distribution and seasonality. Overall, there is a good agreement among the inversions for the mean global total emission, which ranges from 16.1 to 18.7 Tg N yr−1 and is consistent with previous estimates. Ocean emissions represent between 31% and 38% of the global total compared to widely varying previous estimates of 24% to 38%. Emissions from the northern mid to high latitudes are likely to be more important, with a consistent shift in emissions from the tropics and subtropics to the mid to high latitudes in the Northern Hemisphere; the emission ratio for 0–30° N to 30–90° N ranges from 1.5 to 1.9 compared with 2.9 to 3.0 in previous estimates. The largest discrepancies across inversions are seen for the regions of South and East Asia and for tropical and South America owing to the poor observational constraint for these areas and to considerable differences in the modelled transport, especially inter-hemispheric exchange rates and tropical convection. Estimates of the seasonal cycle in N2O emissions are also sensitive to errors in modelled stratosphere-to-troposphere transport in the tropics and southern extra-tropics. Overall, the results show a convergence in the global and regional emissions compared to previous independent studies.

Description: We conducted simulations using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.5 to study air quality in East and South Asia at a spatial resolution of 20 km × 20 km. We find large discrepancies between two existing emissions inventories: the Regional Emission Inventory in Asia version 2 (REAS) and the Emissions Database for Global Atmospheric Research version 4.2 (EDGAR) at the provincial level in China, with maximum differences up to 500 % for CO emissions, 190 % for NO, and 160 % for primary PM10. Such differences in the magnitude and the spatial distribution of emissions for various species lead to 40–70 % difference in surface PM10 concentrations, 16–20 % in surface O3 mixing ratios, and over 100 % in SO2 and NO2 mixing ratios in the polluted areas of China. Our sensitivity run shows WRF-Chem is sensitive to emissions, with the REAS-based simulation reproducing observed concentrations and mixing ratios better than the EDGAR-based simulation for July 2007. We conduct further model simulations using REAS emissions for January, April, July, and October in 2007 and evaluate simulations with available ground-level observations. The model results show clear regional variations in the seasonal cycle of surface PM10 and O3 over East and South Asia. The model meets the air quality model performance criteria for both PM10 (mean fractional bias, MFB ≤ ± 60 %) and O3 (MFB ≤ ± 15 %) in most of the observation sites, although the model underestimates PM10 over Northeast China in January. The model predicts the observed SO2 well at sites in Japan, while it tends to overestimate SO2 in China in July and October. The model underestimates most observed NO2 in all four months. These findings suggest that future model development and evaluation of emission inventories and models are needed for particulate matter and gaseous pollutants in East and South Asia.