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The GEOS-Chem model has been updated with the SAPRC-11 aromatics chemical mechanism, with the purpose of evaluating global and regional effects of the most abundant aromatics (benzene, toluene, xylenes) on the chemical species important for tropospheric oxidation capacity. The model evaluation based on surface and aircraft observations indicates good agreement for aromatics and ozone. A comparison between scenarios in GEOS-Chem with simplified aromatic chemistry (as in the standard setup, with no ozone formation from related peroxy radicals or recycling of NOx) and with the SAPRC-11 scheme reveals relatively slight changes in ozone, hydroxyl radical, and nitrogen oxides on a global mean basis (1–4 %), although remarkable regional differences (5–20 %) exist near the source regions. NOx decreases over the source regions and increases in the remote troposphere, due mainly to more efficient transport of peroxyacetyl nitrate (PAN), which is increased with the SAPRC aromatic chemistry. Model ozone mixing ratios with the updated aromatic chemistry increase by up to 5 ppb (more than 10 %), especially in industrially polluted regions. The ozone change is partly due to the direct influence of aromatic oxidation products on ozone production rates, and in part to the altered spatial distribution of NOx that enhances the tropospheric ozone production efficiency. Improved representation of aromatics is important to simulate the tropospheric oxidation.

Recent studies have shown that surface ozone (O3) concentrations over Central Eastern China (CEC) have increased significantly during the past decade. We quantified the effects of changes in meteorological conditions and O3 precursor emissions on surface O3 levels over CEC between July 2003 and July 2015 using the GEOS-Chem model. The simulated monthly mean maximum daily 8-h average O3 concentration (MDA8 O3) in July increased by approximately 13.6 %, from 65.5 ± 7.9 ppbv (2003) to 74.4 ± 8.7 ppbv (2015), comparable to the observed results. The change in meteorology led to an increase of MDA8 O3 of 5.8 ± 3.9 ppbv over the central part of CEC, in contrast to a decrease of about −0.8 ± 3.5 ppbv over the eastern part of the region. In comparison, the MDA8 O3 over the central and eastern parts of CEC increased by 3.5 ± 1.4 ppbv and 5.6 ± 1.8 ppbv due to the increased emissions. The increase in regional averaged O3 resulting from the emission increase (4.0 ± 1.9 ppbv) was higher than that caused by meteorological changes (3.1 ± 4.9 ppbv) relative to the 2003 standard simulation, while the regions with larger O3 increases showed a higher sensitivity to meteorological conditions than to emission changes. Sensitivity tests indicate that increased levels of anthropogenic non-methane volatile organic compounds (NMVOCs) dominate the O3 increase over the eastern part of CEC, and anthropogenic nitrogen oxides (NOx) mainly increase O3 concentrations over the central and western parts, while decrease O3 in a few urban areas in the eastern part. Process analysis showed that net photochemical production and meteorological conditions (transport in particular) are two important factors that influence O3 levels over the CEC. The results of this study suggest a need to further assess the effectiveness of control strategies for O3 pollution in the context of regional meteorology, transboundary transport, and anthropogenic emission changes.

Technological advancement in industrializing cities is critical for reducing CO2 emissions while maintaining economic growth., As national efforts to reduce CO2 emissions intensify, policy-makers need increasingly specific, subnational information about the sources of CO2 and the potential reductions and economic implications of different possible policies. This is particularly true in China, a large and economically diverse country that has rapidly industrialized and urbanized and that has pledged under the Paris Agreement that its emissions will peak by 2030. We present new, city-level estimates of CO2 emissions for 182 Chinese cities, decomposed into 17 different fossil fuels, 46 socioeconomic sectors, and 7 industrial processes. We find that more affluent cities have systematically lower emissions per unit of gross domestic product (GDP), supported by imports from less affluent, industrial cities located nearby. In turn, clusters of industrial cities are supported by nearby centers of coal or oil extraction. Whereas policies directly targeting manufacturing and electric power infrastructure would drastically undermine the GDP of industrial cities, consumption-based policies might allow emission reductions to be subsidized by those with greater ability to pay. In particular, sector-based analysis of each city suggests that technological improvements could be a practical and effective means of reducing emissions while maintaining growth and the current economic structure and energy system. We explore city-level emission reductions under three scenarios of technological progress to show that substantial reductions (up to 31%) are possible by updating a disproportionately small fraction of existing infrastructure.

Satellite retrieval of vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) is critical for NOx pollution and impact evaluation. For regions with high aerosol loadings, the retrieval accuracy is greatly affected by whether aerosol optical effects are treated implicitly (as additional effective clouds) or explicitly, among other factors. Our previous POMINO algorithm explicitly accounts for aerosol effects to improve the retrieval especially in polluted situations over China, by using aerosol information from GEOS-Chem simulations with further monthly constraint by MODIS/Aqua AOD data. This study updates the retrieval algorithm to POMINO v1.1, by constructing a monthly climatological dataset of aerosol extinction profiles, based on Level-2 CALIOP/CALIPSO data over 2007–2015, to better constrain the modeled aerosol profiles. We find that GEOS-Chem captures the month-to-month variation of CALIOP aerosol layer height but with a systematic underestimate by about 300–600 m (season and location dependent), due to a too strong vertical gradient of extinction above 1 km. Correcting the model aerosol extinction profiles results in small changes in retrieved cloud fraction, increases in cloud top pressure (within 2–6 % in most cases), and increases in tropospheric NO2 VCD by 4–16 % over China on a monthly basis in 2012. The improved NO2 VCDs (in POMINO v1.1) are more consistent with independent ground-based MAX-DOAS observations (R2 = 0.80, NMB = −3.4 %) than POMINO (R2 = 0.80, NMB = −9.6 %) and DOMINO v2 (R2 = 0.68, NMB = −2.1 %) are. Especially on haze days, R2 reaches 0.76 for POMINO v1.1, much higher than that for POMINO (0.68) and DOMINO v2 (0.38). Furthermore, the increase in cloud pressure likely reveals a more realistic vertical relationship between cloud and aerosol layers, with aerosols situated above the clouds in certain months instead of always below the clouds. Our POMINO v1.1 algorithm will be applied to the recently launched TropOMI sensor.

Eastern China (27° N–41° N, 110° E–123° E) is heavily polluted by nitrogen dioxide (NO2), particulate matter with aerodynamic diameter below 2.5 μm (PM2.5) and other air pollutants. These pollutants vary in a variety of temporal and spatial scales, with many temporal scales non-periodic and non-stationary, challenging proper quantitative characterization and visualization. This study uses a newly compiled EOF-EEMD analysis-visualization package to evaluate the spatiotemporal variability of ground-level NO2, PM2.5, and their associations with meteorological processes over Eastern China in Fall–Winter 2013. Applying the package to observed hourly pollutant data reveals a primary spatial pattern representing Eastern China-wide synchronous variation in time, which is dominated by diurnal variability with a much weaker day-to-day signal. A secondary spatial mode, representing north-south opposing changes in time with no constant period, is characterized by wind-related dilution or buildup of pollutants from one day to another. We further evaluate simulations of GEOS-Chem and WRF/CMAQ in capturing the spatiotemporal variability of pollutants. GEOS-Chem underestimates NO2 by about 17 μg/m3 and PM2.5 by 35 μg/m3 on average. It reproduces the diurnal variability for both pollutants. For the day-to-day variation, GEOS-Chem reproduces the observed north-south contrasting mode for both pollutants but not the Eastern China-synchronous mode (especially for NO2). The model errors are due to a first model layer too thick (about 130 m) to capture the near-surface vertical gradient, deficiencies in the nighttime nitrogen chemistry in the first layer, and missing secondary organic aerosols and anthropogenic dusts. CMAQ overestimates the diurnal cycle of pollutants due to too weak boundary layer mixing – especially in the nighttime, CMAQ overestimates NO2 by about 30 μg/m3 and PM2.5 by 60 μg/m3. For the day-to-day variability, CMAQ reproduces the observed Eastern-China synchronous mode but not the north-south opposing mode of NO2. Both models capture the day-to-day variability of PM2.5 better than that of NO2. These results shed light on model improvement. The EOF-EEMD package is freely accessible.

Small-scale nonlinear chemical and physical processes over pollution source regions affect the tropospheric ozone (O3), but these processes are not captured by current global chemical transport models (CTMs) and chemistry–climate models that are limited by coarse horizontal resolutions (100–500 km, typically 200 km). These models tend to contain large (and mostly positive) tropospheric O3 biases in the Northern Hemisphere. Here we use the recently built two-way coupling system of the GEOS-Chem CTM to simulate the regional and global tropospheric O3 in 2009. The system couples the global model (at 2.5° long. × 2° lat.) and its three nested models (at 0.667° long. × 0.5° lat.) covering Asia, North America and Europe, respectively. Specifically, the nested models take lateral boundary conditions (LBCs) from the global model, better capture small-scale processes and feed back to modify the global model simulation within the nested domains, with a subsequent effect on their LBCs. Compared to the global model alone, the two-way coupled system better simulates the tropospheric O3 both within and outside the nested domains, as found by evaluation against a suite of ground (1420 sites from the World Data Centre for Greenhouse Gases (WDCGG), the United States National Oceanic and Atmospheric Administration (NOAA) Earth System Research Laboratory Global Monitoring Division (GMD), the Chemical Coordination Centre of European Monitoring and Evaluation Programme (EMEP), and the United States Environmental Protection Agency Air Quality System (AQS)), aircraft (the High-performance Instrumented Airborne Platform for Environmental Research (HIAPER) Pole-to-Pole Observations (HIPPO) and Measurement of Ozone and Water Vapor by Airbus In- Service Aircraft (MOZAIC)) and satellite measurements (two Ozone Monitoring Instrument (OMI) products). The two-way coupled simulation enhances the correlation in day-to-day variation of afternoon mean surface O3 with the ground measurements from 0.53 to 0.68, and it reduces the mean model bias from 10.8 to 6.7 ppb. Regionally, the coupled system reduces the bias by 4.6 ppb over Europe, 3.9 ppb over North America and 3.1 ppb over other regions. The two-way coupling brings O3 vertical profiles much closer to the HIPPO (for remote areas) and MOZAIC (for polluted regions) data, reducing the tropospheric (0–9 km) mean bias by 3–10 ppb at most MOZAIC sites and by 5.3 ppb for HIPPO profiles. The two-way coupled simulation also reduces the global tropospheric column ozone by 3.0 DU (9.5 %, annual mean), bringing them closer to the OMI data in all seasons. Additionally, the two-way coupled simulation also reduces the global tropospheric mean hydroxyl radical by 5 % with improved estimates of methyl chloroform and methane lifetimes. Simulation improvements are more significant in the Northern Hemisphere, and are mainly driven by improved representation of spatial inhomogeneity in chemistry/emissions. Within the nested domains, the two-way coupled simulation reduces surface ozone biases relative to typical GEOS-Chem one-way nested simulations, due to much improved LBCs. The bias reduction is 1–7 times the bias reduction from the global to the one-way nested simulation. Improving model representations of small-scale processes is important for understanding the global and regional tropospheric chemistry.

Satellite retrievals of vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) normally do not explicitly account for aerosol optical effects and surface reflectance anisotropy that vary with space and time. Here, we conduct an improved retrieval of NO2 VCDs over China, called the POMINO algorithm, based on measurements from the Ozone Monitoring Instrument (OMI), and we test the importance of a number of aerosol and surface reflectance treatments in this algorithm. POMINO uses a parallelized LIDORT-driven AMFv6 package to derive tropospheric air mass factors via pixel-specific radiative transfer calculations with no look-up tables, taking slant column densities from DOMINO v2. Prerequisite cloud optical properties are derived from a dedicated cloud retrieval process that is fully consistent with the main NO2 retrieval. Aerosol optical properties are taken from GEOS-Chem simulations constrained by MODIS aerosol optical depth (AOD) data. MODIS bi-directional reflectance distribution function (BRDF) data are used for surface reflectance over land. For the present analysis, POMINO level-2 data for 2012 are aggregated into monthly means on a 0.25° long. × 0.25° lat. grid. POMINO-retrieved annual mean NO2 VCDs vary from 15–25 × 1015 cm−2 over the polluted North China Plain (NCP) to below 1015 cm−2 over much of western China. Using POMINO to infer Chinese emissions of nitrogen oxides leads to annual anthropogenic emissions of 9.05 TgN yr−1, an increase from 2006 (Lin, 2012) by about 19 %. Replacing the MODIS BRDF data with the OMLER v1 monthly climatological albedo data affects NO2 VCDs by up to 40 % for certain locations and seasons. The effect on constrained NOx emissions is small. Excluding aerosol information from the retrieval process (this is the traditional "implicit" treatment) enhances annual mean NO2 VCDs by 15–40 % over much of eastern China. Seasonally, NO2 VCDs are reduced by 10–20 % over parts of the NCP in spring and over northern China in winter, despite the general enhancements in summer and fall. The effect on subsequently constrained annual emissions is between −5 and +30 % with large seasonal and spatial dependence. The implicit aerosol treatment also tends to exclude days with high pollution, since aerosols are interpreted as effective clouds and the respective OMI pixels are often excluded by cloud screening; this is a potentially important sampling bias. Therefore an explicit treatment of aerosols is important for space-based NO2 retrievals and emission constraints. A comprehensive independent measurement network with sufficient spatial and temporal representativeness is needed to further evaluate the different satellite retrieval approaches.

Epidemiological and health impact studies of fine particulate matter (PM 2.5 ) have been limited in China because of the lack of spatially and temporally continuous PM 2.5 monitoring data. Satellite remote sensing of aerosol optical depth (AOD) is widely used in estimating ground-level PM 2.5 concentrations. We improved the method for estimating long-term surface PM 2.5 concentrations using satellite remote sensing and a chemical transport model, and derived PM 2.5 concentrations over China for 2006–2012. We generated a map of surface PM 2.5 concentrations at 0.1° × 0.1° over China using the nested-grid GEOS-Chem model, most recent bottom-up emission inventory, and satellite observations from the MODIS and MISR instruments. Aerosol vertical profiles from the space-based CALIOP lidar were used to adjust the climatological drivers of the bias in the simulated results, and corrections were made for incomplete sampling. We found significant spatial agreement between the satellite-derived PM 2.5 concentrations and the ground-level PM 2.5 measurements collected from literatures (r = 0.74, slope = 0.77, intercept = 11.21 μg/m 3 ). The population-weighted mean of PM 2.5 concentrations in China is 71 μg/m 3 and more than one billion people live in locations where PM 2.5 concentrations exceed the World Health Organization Air Quality Interim Target-1 of 35 μg/m 3 . The results from our work are substantially higher than previous work, especially in heavily polluted regions. The overall population-weighted mean uncertainty over China is 17.2 μg/m 3 , as estimated using ground-level AOD measurements and vertical profiles observed from CALIOP.

Reaction of quinolone type antibiotics (enrofloxacin, ciprofloxacin, norfloxacin and ofloxacin) with lanthanide ions (Eu3+ and Tb3+) afforded eight kinds of complexes that can be dissolved in water. These compounds possess not only the advantages of long excited state lifetimes, but also allow excitation in the visible light range depending on the concentration variation. Especially the excitation wavelength of the terbium complexes can be extended into 405 nm. Theoretical studies demonstrated that the calculated energy gaps between HOMO and LUMO+1 orbital could be reduced and a dimeric structure was formed during the concentration experiments. Moreover, uniform and long rod-like structures (diameter: 100 nm; length: 10 μm) were achieved and concentration dependence has been investigated. The strategy of combining lanthanide characteristic emission nature and longer wavelength excitations can be applicable to the development of luminescent devices with controllable shapes.

High-voltage cathode material LiNi0.5Mn1.5O4 has been first synthesized by a novel metal-cholated supramolecular hydrogel as precursor. The structural analysis was investigated by X-ray powder diffraction, scanning electronic microscope, and Fourier transform infrared spectroscopy. The results indicated that the as-products possessed well constructed spinel structure and high crystallinity and pure phase through adding optimal amount of cholic acid. The electrochemical properties were also investigated, and its results showed that the LiNi0.5Mn1.5O4 material exhibited enhanced rate capacity and cycling properties as electrode materials in lithium cells mainly due to the improved crystallinity and higher pure phase. In a word, this new approach provides an alternative and promising route for the fabrication of cathode materials with perfect octahedron structure and excellent electrochemical properties using metal-driven hydrogels as template.

Substantial anthropogenic emissions from China have resulted in serious air pollution, and this has generated considerable academic and public concern. The physical transport of air pollutants in the atmosphere has been extensively investigated; however, understanding the mechanisms how the pollutant was transferred through economic and trade activities remains a challenge. For the first time, we quantified and tracked China's air pollutant emission flows embodied in interprovincial trade, using a multiregional input–output model framework. Trade relative emissions for four key air pollutants (primary fine particle matter, sulfur dioxide, nitrogen oxides and non-methane volatile organic compounds) were assessed for 2007 in each Chinese province. We found that emissions were significantly redistributed among provinces owing to interprovincial trade. Large amounts of emissions were embodied in the imports of eastern regions from northern and central regions, and these were determined by differences in regional economic status and environmental policy. It is suggested that measures should be introduced to reduce air pollution by integrating cross-regional consumers and producers within national agreements to encourage efficiency improvement in the supply chain and optimize consumption structure internationally. The consumption-based air pollutant emission inventory developed in this work can be further used to attribute pollution to various economic activities and final demand types with the aid of air quality models.

China emits a considerable amount of air pollutants when producing goods for export. Previous efforts have emphasized the magnitude of export-related emissions; however, their health consequences on the Chinese population have not been quantified. Here, we present an interdisciplinary study to estimate the health impact of export-related air pollution. The results show that export-related emissions elevated the annual mean population weighted PM2.5 by 8.3 μg/m(3) (15% of the total) in 2007, causing 157,000 deaths and accounting for 12% of the total mortality attributable to PM2.5-related air pollution. Compared to the eastern coastal provinces, the inner regions experience much larger export-related health losses relative to their economic production gains, owing to huge inter-regional disparities in export structures and technology levels. A shift away from emission-intensive production structure and export patterns, especially in inner regions, could significantly help improve national exports while alleviating the inter-regional cost-benefit inequality. Our results provide the first quantification of health consequences from air pollution related to Chinese exports. The proposed policy recommendations, based on health burden, economic production gains, and emission analysis, would be helpful to develop more sustainable and effective national and regional export strategies.

The Fukushima Nuclear Accident (FNA) resulted in a large amount of radionuclides released into the atmosphere and dispersed globally, which has greatly raised public concerns. The state of the art for source terms of 19 kinds of radionuclides derived from the FNA was comprehensively collected and compared with levels of the global fallout and the Chernobyl Nuclear Accident (CNA). The atmospheric impacts of the FNA were evaluated from three aspects including radioactive baseline of the atmosphere, the concentration limits in standards and radiological protection. The FNA should not impose significant radiological risk on the public members in the countries excluding Japan. A conceptual scheme of Fukushima-derived radionuclides with physical and physicochemical insights on different temporal–spatial timescales was discussed and illustrated to understand their fates in the atmosphere.

Rapid industrialization in Asia in the last two decades has resulted in a significant increase in Asian ozone (O3) precursor emissions with likely a corresponding increase in the export of O3 and its precursors. However, the relationship between this increasing O3, the chemical environment, O3 production efficiency, and the partitioning between anthropogenic and natural precursors is unclear. In this work, we use satellite measurements of O3, CO and NO2 from TES (Tropospheric Emission Spectrometer), MOPITT (Measurement of Pollution In The Troposphere) and OMI (Ozone Monitoring Instrument) to quantify O3 precursor emissions for 2006 and their impact on free tropospheric O3 over northeastern Asia, where pollution is typically exported globally due to strong westerlies. Using the GEOS-Chem (Goddard Earth Observing System Chemistry) global chemical transport model, we test the modeled seasonal and interannual variation of O3 based on prior and updated O3 precursor emissions where the updated emissions of CO and NOx are based on satellite measurements of CO and NO2. We show that the observed TES O3 variability and amount are consistent with the model for these updated emissions. However, there is little difference in the modeled ozone between the updated and prior emissions. For example, for the 2006 June time period, the prior and posterior NOx emissions were 14% different over China but the modeled ozone in the free troposphere was only 2.5% different. Using the adjoint of GEOS-Chem we partition the relative contributions of natural and anthropogenic sources to free troposphere O3 in this region. We find that the influence of lightning NOx in the summer is comparable to the contribution from surface emissions but smaller for other seasons. China is the primary contributor of anthropogenic CO, emissions and their export during the summer. While the posterior CO emissions improved the comparison between model and TES by 32%, on average, this change also had only a small effect on the free tropospheric ozone. Our results show that the influence of India and southeastern Asia emissions on O3 pollution export to the northwestern Pacific is sizeable, comparable with Chinese emissions in winter, about 50% of Chinese emissions in spring and fall, and approximately 20% of the emissions in the summer.

A novel luminescent organic-inorganic hybrid terbium material containing a boronic acid receptor site has been designed and synthesized. Ultra-violet excitation of the material results in green emission from the terbium core. Homogenous spherical nanoparticles with the average diameter of 60 nm were achieved by embedding the terbium complex onto a silica surface. The boron–fluoride interactions of the new material in an aqueous environment provide for a new on-off luminescence sensor for fluoride ions in the field of lanthanide based multifunctional materials.

The design, synthesis, photophysical properties and practical application of fluorescent silicon nanoparticles (SiNPs) of a quantum-size (∼3 nm) have been studied. 3-Aminopropyltrimethoxysilane (APTMS) and 3-aminopropyltriethoxysilane (APTES) were employed as sources. The newly developed nanoparticles show excellent water solubility and luminescent features. Herein we report a novel chemical approach for selective tetracycline (TC) recognition and a new type of targetable fluorescent sensor has been prepared. The blue emission, peaking at 440 nm, was dramatically quenched in the presence of TCs. Moreover, we utilized this probe in a milk sample study for the determination of TCs, demonstrating its advantages of simplicity and practicality.

Surface-based measurements from the EMEP network are used to estimate the changes in surface ozone levels during the 1995–2014 period over Europe. It is shown that a significantly decreasing trend in the 95th percentile ozone concentrations has occurred, especially during noontime (0.9 µg/m3/y), while the 5th percentile ozone concentrations continued to increase with a trend of 0.3 µg/m3/y during the study period. With the help of numerical simulations performed with the global chemistry-climate model EMAC, the importance of anthropogenic emissions changes in determining these changes are investigated. The EMAC model is found to successfully capture the observed temporal variability in mean ozone concentrations, as well as the contrast in the trends of 95th and 5th percentile ozone over Europe. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels, and that background ozone levels have been influenced by hemispheric transport, while climate variability generally regulated the inter-annual variations of surface ozone in Europe.

Models severely overestimate surface ozone in the Southeast US during summertime and this overestimation has implications for the design of air quality regulations. We use the GEOS-Chem model to interpret ozone observations from aircraft (SEAC4RS), ozonesondes (SEACIONS), and surface sites (CASTNET) in August–September 2013. After correcting for a 30–50 % NOx emission overestimate in the US EPA National Emission Inventory, we find that the model is unbiased relative to aircraft observations below 1 km. However, surface observations of maximum daily 8-h average (MDA8) ozone are still biased high in the model (averaging 48 ± 9 ppb) compared to observations (40 ± 9 ppb). The low tail in the observations (MDA8 ozone

Millions of people die every year from diseases caused by exposure to outdoor air pollution1, 2, 3, 4, 5. Some studies have estimated premature mortality related to local sources of air pollution6, 7, but local air quality can also be affected by atmospheric transport of pollution from distant sources8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18. International trade is contributing to the globalization of emission and pollution as a result of the production of goods (and their associated emissions) in one region for consumption in another region14, 19, 20, 21, 22. The effects of international trade on air pollutant emissions23, air quality14 and health24 have been investigated regionally, but a combined, global assessment of the health impacts related to international trade and the transport of atmospheric air pollution is lacking. Here we combine four global models to estimate premature mortality caused by fine particulate matter (PM2.5) pollution as a result of atmospheric transport and the production and consumption of goods and services in different world regions. We find that, of the 3.45 million premature deaths related to PM2.5 pollution in 2007 worldwide, about 12 per cent (411,100 deaths) were related to air pollutants emitted in a region of the world other than that in which the death occurred, and about 22 per cent (762,400 deaths) were associated with goods and services produced in one region for consumption in another. For example, PM2.5 pollution produced in China in 2007 is linked to more than 64,800 premature deaths in regions other than China, including more than 3,100 premature deaths in western Europe and the USA; on the other hand, consumption in western Europe and the USA is linked to more than 108,600 premature deaths in China. Our results reveal that the transboundary health impacts of PM2.5 pollution associated with international trade are greater than those associated with long-distance atmospheric pollutant transport.

Air quality is a major environmental concern in China, where premature deaths due to air pollution exceed 1 million people per year in recent years. Here, using a novel coupling of economic, physical and epidemiological models, we estimate the premature mortality in seven regions of China related to emissions of PM2.5 and precursor gases in 2010 and show for the first time how the distribution of these deaths in China is determined by a combination of economic activities and physical transport of pollution in the atmosphere. We find that 33 % of China’s air pollution deaths in 2010 were caused by pollutants emitted in a different region of the country and transported in the atmosphere, especially from north to south and from east to west. Similarly, 38 % of deaths were related to goods and services consumed in a different region from where they were produced. For example, 36 % of the deaths number associated to emissions in Central region of China were caused by consumption in other regions. As a combined result from atmospheric transport and trade, 56 % of pollution deaths in China were related to consumption in a different region. Among these, 14 % of China’s pollution deaths were caused by international export. Our results indicate that multilateral and multi-stage cooperation under a regional sustainable development framework is in urgent need to mitigate air pollution and health impacts, and efforts to reduce the health impacts of air pollution in China should be prioritized according to the source and location of emissions, the type and economic value of the emitting activities, and the related patterns of consumption.

Despite much effort made in studying human health associated with fine particulate matter (PM2.5), our knowledge about PM2.5 and human health from a long-term perspective is still limited by inadequately long data. Here, we presented a novel method to retrieve surface PM2.5 mass concentrations using surface visibility measurements and GEOS-Chem model simulations. First, we used visibility measurements and the ratio of PM2.5 and aerosol extinction coefficient (AEC) in GEOS-Chem to calculate visibility-inferred PM2.5 at individual stations (SC-PM2.5). Then we merged SC-PM2.5 with the spatial pattern of GEOS-Chem modeled PM2.5 to obtain a gridded PM2.5 dataset (GC-PM2.5). We validated the GC-PM2.5 data over the North China Plain on a 0.3125° longitude x 0.25° latitude grid in January, April, July and October 2014, using ground-based PM2.5 measurements. The spatial patterns of temporally averaged PM2.5 mass concentrations are consistent between GC-PM2.5 and measured data with a correlation coefficient of 0.79 and a linear regression slope of 0.8. The spatial average GC-PM2.5 data reproduce the day-to-day variation of observed PM2.5 concentrations with a correlation coefficient of 0.96 and a slope of 1.0. The mean bias is less than 12 μg/m3 (

Horizontal visibility measured at ground meteorological stations provides an under-exploited source of information for studying the interdecadal variation of aerosols and their climatic impacts. Here we propose to use a 3-hourly visibility dataset to infer aerosol optical depth (AOD) over East China, using the nested GEOS-Chem chemical transport model to interpret the spatiotemporally varying relations between columnar and near-surface aerosols. Our analysis is focused in 2006 under cloud-free conditions. We evaluate the visibility-inferred AOD using MODIS/Terra and MODIS/Aqua AOD datasets, after validating MODIS data against three ground AOD measurement networks (AERONET, CARSNET and CSHNET). We find that the two MODIS datasets agree with ground-based AOD measurements, with negative mean biases of 0.05–0.08 and Reduced Major Axis regression slopes around unity. Visibility-inferred AOD roughly capture the general spatiotemporal patterns of the two MODIS datasets with negligible mean differences. The inferred AOD reproduce the seasonal variability (correlation exceeds 0.9) and the slight AOD growth from the late morning to early afternoon shown in the MODIS datasets, suggesting the validity of our AOD inference method. Future research will extend the visibility-based AOD inference to study the long-term variability of AOD.

The concept of “slow release anions for the assembly of crystals” was successfully carried out through a facile, effective and environmental friendly supersonic and microwave co-assistance (SMC) approach at very low temperature in less than 40 min. It has been found that the rational design of multiple irradiations, lanthanide contraction and fluoride sources would make it possible to control both the crystalline phases (hexagonal or orthorhombic) and the microstructures (including nanoparticles, nanoplates or micro-meter scale particles). The photo-luminescent properties of EuF 3 and TbF 3 revealed that characteristic red and green emissions can be excited by multiple wavelengths. Moreover, the results demonstrated that there are efficient energy transfers from Gd 3+ to Eu 3+ and Tb 3+ in GdF 3 : Eu 3+ and GdF 3 : Tb 3+ phosphors based on this new method.

Retrievals of tropospheric nitrogen dioxide (NO2) from the Ozone Monitoring Instrument (OMI) are subject to errors in the treatments of aerosols, surface reflectance anisotropy, and vertical profile of NO2. Here we quantify the influences over China via an improved retrieval process. We explicitly account for aerosol optical effects (simulated by nested GEOS-Chem at 0.667° long. × 0.5° lat. and constrained by aerosol measurements), surface reflectance anisotropy, and high-resolution vertical profiles of NO2 (simulated by GEOS-Chem). Prior to the NO2 retrieval, we derive the cloud information using consistent ancillary assumptions. We compare our retrieval to the widely used DOMINO v2 product, using MAX-DOAS measurements at three urban/suburban sites in East China as reference and focusing the analysis on the 127 OMI pixels (in 30 days) closest to the MAX-DOAS sites. We find that our retrieval reduces the interference of aerosols on the retrieved cloud properties, thus enhancing the number of valid OMI pixels by about 25%. Compared to DOMINO v2, our retrieval better captures the day-to-day variability in MAX-DOAS NO2 data (R2 = 0.96 versus 0.72), due to pixel-specific radiative transfer calculations rather than the use of a look-up table, explicit inclusion of aerosols, and consideration of surface reflectance anisotropy. Our retrieved NO2 columns are 54% of the MAX-DOAS data on average, reflecting the inevitable spatial inconsistency between the two types of measurement, errors in MAX-DOAS data, and uncertainties in our OMI retrieval related to aerosols and vertical profile of NO2. Sensitivity tests show that excluding aerosol optical effects can either increase or decrease the retrieved NO2 for individual OMI pixels with an average increase by 14%. Excluding aerosols also complexly affects the retrievals of cloud fraction and particularly cloud pressure. Employing various surface albedo data sets slightly affects the retrieved NO2 on average (within 10%). The retrieved NO2 columns increase when the NO2 profiles are taken from MAX-DOAS retrievals (by 19% on average) or TM4 simulations (by 13%) instead of GEOS-Chem simulations. Our findings are also relevant to retrievals of other pollutants (e.g., sulfur dioxide, ormaldehyde, glyoxal) from UV–visible backscatter satellite instruments.

A novel supersonic microwave co-assistance method (abbreviated as SMC) was used to efficiently synthesize BaMO4: Ln3+ (M = W, Mo; Ln = Eu, Tb) red/green phosphors at low temperature (343 K) in 40 min. X-ray powder diffraction (abbreviated as XRD), scanning electronic microscope (abbreviated as SEM) and photoluminescent spectra techniques (abbreviated as PL) were used to characterize the phosphors. SEM images revealed that shuttle shaped structures were achieved. The fluorescence property of phosphors demonstrated that both BaWO4 and BaMoO4 are efficient matrixes to sensitize europium or terbium. The red/green emissions were greatly enhanced under the simultaneous supersonic and microwave irradiation. We considered that this facile and effective technique owns the advantages of saving energy and shortening reaction time in contrast to conventional methods which may be promising in fabricating luminescent materials.

In this paper, phosphors of LuF 3 :Eu 3+ /Tb 3+ have been successfully synthesized with small chelator ethylenediaminetetra acetic acid (EDTA) or amphiphilic polymer (polyethylene glycol, PEG-1000) as templates via a hydrothermal method. X-ray powder diffraction (XRD), scanning electronic microscope (SEM), and photo-luminescent spectra techniques (PL) were used to characterize the as-prepared samples. XRD patterns showed that well crystallized lanthanide fluorides with hexagonal phase were achieved. SEM images revealed that different regular microstructures were achieved. The photo-luminescent properties of LuF 3 :Eu 3+ demonstrated that there are significant energy transfers from fluorides to Eu 3+ . The results presented that EDTA as the template will lead to the highest emission intensities.

Two different methods (hydrothermal and supersonic microwave co-assistance (SMC)) were used to assemble a novel phosphor CdMoO4:Eu3+. X-ray powder diffraction (XRD), scanning electronic microscope (SEM), and photoluminescent spectra (PL) were applied to characterize the target samples. SEM images revealed that olive-like and spherical shape of the micro-structures were controllable in terms of the two approaches. The fluorescence spectra demonstrate energy transfer from MoO 4 2 - to Eu3+ and the red emission was greatly enhanced under the irradiations of SMC. The photo-catalytic activity of CdMoO4:Eu3+ was investigated by the photo-degradation of rhodamine B.

GdNbO 4 :Eu 3+ and LuTaO 4 :Eu 3+ have been successfully prepared with different fluxes (NaCl, KCl, NaCl and KCl) by the molten salt method. X-ray diffraction (XRD) patterns illustrated that well crystallized GdNbO 4 :Eu 3+ and LuTaO 4 :Eu 3+ in the presence of fluxes were formed under reduced temperature (900 °C) in contrast to conventional method (GdNbO 4 :Eu 3+ : around 1200 °C; LuTaO 4 :Eu 3+ : around 1500 °C). Scanning electron microscope (SEM) images revealed that well dispersed particles were achieved (granular or rod-like structures). Meanwhile, the photo-luminescent studies demonstrated that both niobate and tantalate are efficient hosts to sensitize europium red emissions. The results indicated that GdNbO 4 :Eu 3+ using NaCl as the flux gave much enhanced red emission whereas LuTaO 4 :Eu 3+ synthesized with the assistance of mixed salts (NaCl–KCl) achieved the best luminescence.

Errors in chemical transport models (CTMs) interpreting the relation between space-retrieved tropospheric column densities of nitrogen dioxide (NO2) and emissions of nitrogen oxides (NOx) have important consequences on the inverse modeling. They are however difficult to quantify due to lack of adequate in situ measurements, particularly over China and other developing countries. This study proposes an alternate approach for model evaluation over East China, by analyzing the sensitivity of modeled NO2 columns to errors in meteorological and chemical parameters/processes important to the nitrogen abundance. As a demonstration, it evaluates the nested version of GEOS-Chem driven by the GEOS-5 meteorology and the INTEX-B anthropogenic emissions and used with retrievals from the Ozone Monitoring Instrument (OMI) to constrain emissions of NOx. The CTM has been used extensively for such applications. Errors are examined for a comprehensive set of meteorological and chemical parameters using measurements and/or uncertainty analysis based on current knowledge. Results are exploited then for sensitivity simulations perturbing the respective parameters, as the basis of the following post-model linearized and localized first-order modification. It is found that the model meteorology likely contains errors of various magnitudes in cloud optical depth, air temperature, water vapor, boundary layer height and many other parameters. Model errors also exist in gaseous and heterogeneous reactions, aerosol optical properties and emissions of non-nitrogen species affecting the nitrogen chemistry. Modifications accounting for quantified errors in 10 selected parameters increase the NO2 columns in most areas with an average positive impact of 18% in July and 8% in January, the most important factor being modified uptake of the hydroperoxyl radical (HO2) on aerosols. This suggests a possible systematic model bias such that the top-down emissions will be overestimated by the same magnitude if the model is used for emission inversion without corrections. The modifications however cannot eliminate the large model underestimates in cities and other extremely polluted areas (particularly in the north) as compared to satellite retrievals, likely pointing to underestimates of the a priori emission inventory in these places with important implications for understanding of atmospheric chemistry and air quality. Note that these modifications are simplified and should be interpreted with caution for error apportionment.

Herein, a novel fluorescent indicator for the real-time monitoring of amines is described. This probe contains a complex of europium-(thenoyltrifluoroacetone)3 (Eu(TTA)3) that efficiently reacts with primary and secondary amines. The electronwithdrawing trifluoroacetyl undergoes a nucleophilic addition with amines, and the complex was used to selectively detect BuNH2 and Et2NH (quenching concentration for BuNH2: 10 )4 M, for Et2NH: 1.2 · 10 )3 M) by monitoring emission; no changes were observed in the emission spectrum of Eu(TTA)3 in the presence of Et3N, [Bu4N]Cl, or PhNH2 in aqueous solution (THF ⁄ H2O = 1:1). The ratio of emission intensity to amine concentration was linear by the least-squares fitting method.

Vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) retrieved from space provide valuable information to estimate emissions of nitrogen oxides (NOx) inversely. Accurate emission attribution to individual sources, important both for understanding the global biogeochemical cycling of nitrogen and for emission control, remains difficult. This study presents a regression-based multi-step inversion approach to estimate emissions of NOx from anthropogenic, lightning and soil sources individually for 2006 over East China on a 0.25° long × 0.25° lat grid, employing the DOMINO product version 2 retrieved from the Ozone Monitoring Instrument. The inversion is done gridbox by gridbox to derive the respective emissions, taking advantage of differences in seasonality between anthropogenic and natural sources. Lightning and soil emissions are combined together for any given gridbox due to their similar seasonality; and their different spatial distributions are used implicitly for source separation to some extent. The nested GEOS-Chem model for East Asia is used to simulate the seasonal variations of different emission sources and impacts on VCDs of NO2 for the inversion purpose. Sensitivity tests are conducted to evaluate key assumptions embedded in the inversion process. The inverse estimate suggests annual budgets of about 7.1 TgN (±39%), 0.21 TgN (±61%), and 0.38 TgN (±65%) for the a posteriori anthropogenic, lightning and soil emissions, respectively, about 18–23% higher than the respective a priori values. The enhancements in anthropogenic emissions are largest in cities and areas with extensive use of coal, particularly in the north in winter, as evident on the high-resolution grid. Derived soil emissions are consistent with recent bottom-up estimates. They are less than 6% of anthropogenic emissions annually, increasing to about 13% for July. Derived lightning emissions are about 3% of anthropogenic emissions annually and about 10% in July. Overall, anthropogenic emissions are found to be the dominant source of NOx over East China with important implications for nitrogen control.

Rapid economic and industrial development in China and relatively weak emission controls have resulted in significant increases in emissions of nitrogen oxides (NOx) in recent years, with the exception of late 2008 to mid 2009 when the economic downturn led to emission reductions detectable from space. Here vertical column densities (VCDs) of tropospheric NO2 retrieved from satellite observations by SCIAMACHY, GOME-2 and OMI (both by KNMI and by NASA) are used to evaluate changes in emissions of NOx from October 2004 to February 2010 identifying impacts of the economic downturn. Data over polluted regions of Northern East China suggest an increase of 27–33 % in 12-month mean VCD of NO2 prior to the downturn, consistent with an increase of 49 % in thermal power generation (TPG) reflecting the economic growth. More detailed analysis is used to quantify changes in emissions of NOx in January over the period 2005–2010 when the effect of the downturn was most evident. The GEOS-Chem model is employed to evaluate the effect of changes in chemistry and meteorology on VCD of NO2. This analysis indicates that emissions decreased by 20 % from January 2008 to January 2009, close to the reduction of 18 % in TPG that occurred over the same interval. A combination of three independent approaches indicates that the economic downturn was responsible for a reduction in emissions by 9–11 % in January 2009 with an additional decrease of 10 % attributed to the slow-down in industrial activity associated with the coincident celebration of the Chinese New Year; errors in the estimate are most likely less than 3.4 %.

Lanthanide tris(2-thenoyltrifluoroacetonate) complex based on 2-(3,5-difluorophenyl)imidazo [4,5-f]-1,10-phenanthroline (1) with red luminescence acted as effective receptors for F− and AcO− anions. Spectroscopic studies of UV–vis, fluorescence and NMR present that the sensor exhibits striking emission changes to fluoride (green) and acetate anions (yellow-red to green) respectively due to hydrogen binding interactions. More importantly, transparent hybrid thick films composed by europium complex and poly-methyl methacrylate (PMMA) matrix were successfully prepared. All the films exhibit intense red emissions of europium ions and the optimized composing concentration of luminescent species is 0.5 mg/5 ml MMA. The derived film could give rise to luminescence change in fluoride anion containing DMSO solution. The micro-structure and size of the hybrid films were characterized by dynamic light scattering (DLS), the results reflect that granule size has the average diameter of 300 nm.

The study aims were to investigate the correlation between vertebral shape and hand-wrist maturation and to select characteristic parameters of C2-C5 (the second to fifth cervical vertebrae) for cervical vertebral maturation determination by mixed longitudinal data. 87 adolescents (32 males, 55 females) aged 8-18 years with normal occlusion were studied. Sequential lateral cephalograms and hand-wrist radiographs were taken annually for 6 consecutive years. Lateral cephalograms were divided into 11 maturation groups according to Fishman Skeletal Maturity Indicators (SMI). 62 morphological measurements of C2-C5 at 11 different developmental stages (SMI1-11) were measured and analysed. Locally weighted scatterplot smoothing, correlation coefficient analysis and variable cluster analysis were used for statistical analysis. Of the 62 cervical vertebral parameters, 44 were positively correlated with SMI, 6 were negatively correlated and 12 were not correlated. The correlation coefficients between cervical vertebral parameters and SMI were relatively high. Characteristic parameters for quantitative analysis of cervical vertebral maturation were selected. In summary, cervical vertebral maturation could be used reliably to evaluate the skeletal stage instead of the hand-wrist radiographic method. Selected characteristic parameters offered a simple and objective reference for the assessment of skeletal maturity and timing of orthognathic surgery.

Mixing in the planetary boundary layer (PBL) affects vertical distributions of air tracers in the lower troposphere. An accurate representation of PBL mixing is critical for chemical-transport models (CTMs) for applications sensitive to simulations of the vertical profiles of tracers. The full mixing assumption in the widely used global CTM GEOS-Chem has recently been supplemented with a non-local PBL scheme. This study analyzes the impact of the non-local scheme on model representation of PBL mixing, consequences for simulations of vertical profiles of air tracers and surface air pollution, and implications for model applications to the interpretation of data retrieved from satellite remote sensing. The non-local scheme significantly improves simulations of the vertical distributions for NO2 and O3, as evaluated using aircraft measurements in summer 2004. It also reduces model biases over the U.S. by more than 10 ppb for surface ozone concentrations at night and by 2–5 ppb for peak ozone in the afternoon, as evaluated using ground observations. The application to inverse modeling of anthropogenic NOx emissions for East China using satellite retrievals of NO2 from OMI and GOME-2 suggests that the full mixing assumption results in 3–14% differences in top–down emission budgets as compared to the non-local scheme. The top–down estimate combining the non-local scheme and the Lin et al. inverse modeling approach suggests a magnitude of 6.6 TgN yr−1 for emissions of NOx over East China in July 2008 and 8.0 TgN yr−1 for January 2009, with the magnitude and seasonality in good agreement with bottom–up estimates.

A new methodology is developed to constrain Chinese anthropogenic emissions of nitrogen oxides (NOx) from four major sectors (industry, power plants, mobile and residential) in July 2008. It combines tropospheric NO2 column retrievals from GOME-2 and OMI, taking advantage of their different passing time over China (~10:00 a.m. LT (local time) versus ~02:00 p.m.) and consistent retrieval algorithms. The approach is based on the difference of NOx columns at the overpass times of the two instruments; it thus is less susceptible to the likely systematic errors embedded in individual retrievals that are consistent with each other. Also, it explicitly accounts for diurnal variations and uncertainties of NOx emissions for individual sources. Our best top-down estimate suggests a national budget of 6.8 TgN/yr (5.5 TgN/yr for East China), close to the a priori bottom-up emission estimate from the INTEX-B mission for the year of 2006. The top-down emissions are lower than the a priori near Beijing, in the northeastern provinces and along the east coast; yet they exceed the a priori over many inland regions. Systematic errors in satellite retrievals are estimated to lead to underestimation of top-down emissions by at most 17% (most likely 10%). Effects of other factors on the top-down estimate are typically less than 15% each, including lightning, soil emissions, mixing in planetary boundary layer, anthropogenic emissions of carbon monoxide and volatile organic compounds, magnitude of a priori emissions, assumptions on emission diurnal variations, and uncertainties in the four sectors. The a posteriori emission budget is 5.7 TgN/yr for East China.

Future changes in climate and precursor emissions will likely have important consequences on ground-level ozone concentrations for the City of Chicago and its surrounding suburban/rural areas. Here we use a regional climate-air quality modeling system to evaluate the combined and individual effects of climate warming (and resulting biogenic emissions increases) and anthropogenic emissions perturbations from 1996–2000 to 2048– 2052 and 2095–2099 in this region. Two scenarios are considered, including A1FI (higher warming with increasing anthropogenic emissions) and B1 (less warming with reduced anthropogenic emissions). Relative to 1996–2000, projected changes in climate and anthropogenic emissions together lead to little ozone change for the City of Chicago under A1FI but 5.0–7.8 ppb increases under B1 by 2048–2052 and 2095–2099. For A1FI, the decreasing ratio of volatile organic compounds (VOCs) to nitrogen oxides (NOx) reduces ozone concentrations over Chicago, despite the increasing emissions ...

The concept of Global Warming Potentials (GWPs) has been extensively used in policy consideration as a relative index for comparing the climate impact of an emitted greenhouse gas (GHG), relative to carbon dioxide with equal mass emissions. Ozone depletion due to emission of chlorinated or brominated halocarbons leads to cooling of the climate system in the opposite direction to the direct warming contribution by halocarbons as GHGs. This cooling is a key indirect effect of the halocarbons on climatic radiative forcing, which is accounted for by indirect GWPs. With respect to climate, it is critical to understand net influences considering direct warming and indirect cooling effects especially for Halons due to the greater ozone-depleting efficiency of bromine over chlorine. Until now, the indirect GWPs have been calculated using a parameterized approach based on the concept of Equivalent Effective Stratospheric Chlorine (EESC) and the observed ozone depletion over the last few decades. As a step towards obtaining indirect GWPs through a more robust approach, we use atmospheric models to explicitly calculate the indirect GWPs of Halon-1211 and Halon-1301 for a 100-year time horizon. State-of-the-art global chemistry-transport models (CTMs) were used as the computational tools to derive more realistic ozone depletion changes caused by an added pulse emission of the two major Halons at the surface. The radiative forcings on climate from the ozone changes have been calculated for indirect GWPs using an atmospheric radiative transfer model (RTM). The simulated temporal variations of global average total column Halons after a pulse perturbation follow an exponential decay with an e-folding time which is consistent with the expected chemical lifetimes of the Halons. Our calculated indirect GWPs for the two Halons are much smaller than those from past studies but are within a single standard deviation of WMO (2007) values and the direct GWP values derived agree with the published values. Our model-based assessment of the Halon indirect GWPs thus confirms the significant importance of indirect effects on climate.

A discussion of the thickness of current sheets in solar eruptions, d, led Lin et al. in 2007 to estimate very large values for the effective resistivity, eta(e). Here, we address some questions raised by that paper. We apply the limb synoptic map technique and find d between 5.0 x 10(4) and 4.6 x 10(5) km, increasing with both time and altitude. The possibility that large apparent d and eta(e) result from projection effects is examined and rejected. We derive theoretical scaling laws relating d to other observables that corroborate this conclusion and thus help confine both d and eta(e) to a reasonable range. The possible impact of our results on the existing models of particle acceleration in reconnecting current sheets is also briefly discussed.

Simulation of summertime U.S. surface ozone diurnal cycle is influenced by the model representation of planetary boundary layer (PBL) mixing, spatial resolution, and precursor emissions. These factors are investigated here for five major regions (Northeast, Midwest, Southeast, California, and Southwest) by using the Model for Ozone And Related chemical Tracers version 2.4 (MOZART-2.4), with important modifications, to conduct sensitivity experiments for summer 1999 with three PBL mixing schemes, two horizontal resolutions and two emissions datasets. Among these factors, the PBL mixing is dominant. The default non-local scheme well reproduces the observed ozone diurnal variation, where the timing for the afternoon maximum and the morning minimum is within 1 h of the observed; biases for the minimum are less than 5 ppb except over the Southeast; and the ozone maximum–minimum contrast (OMMC) is within 10 ppb of observations except for the overprediction by 18.9 ppb over the Northeast. In contrast, the local scheme significantly overestimates the OMMC by 10–34 ppb over all regions as ozone and precursors are trapped too close to the ground. On the other hand, the full-mixing assumption underestimates the OMMC by 0–25 ppb, except over the Northeast, as the nighttime ozone decline is greatly underpredicted. As compared to PBL mixing, the effects of horizontal resolutions and precursor emissions being used are smaller but non-negligible. Overall, with the non-local mixing scheme, relatively high horizontal resolution (∼1.1°) and updated emissions data, the modified MOZART is capable of simulating the main features of the observed ozone diurnal cycle.

Future projections of near-surface ozone concentrations depend on the climate/emissions scenario used to drive future simulations, the direct effects of the changing climate on the atmosphere, and the indirect effects of changing temperatures and CO2 levels on biogenic ozone precursor emissions. The authors investigate the influence of these factors on potential future changes in summertime daily 8-h maximum ozone over the United States and China by comparing Model for Ozone and Related Chemical Tracers, version 2.4, (MOZART-2.4) simulations for the period 1996–2000 with 2095–99, using climate projections from NCAR–Department of Energy Parallel Climate Model simulations driven by the Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios A1fi (higher) and B1 (lower) emission scenarios, with corresponding changes in biogenic emissions. The effect of projected climate changes alone on surface ozone is generally less than 3 ppb over most regions. Regional ozone increases and decreases are driven mainly by local warming and marine air dilution enhancement, respectively. Changes are approximately the same magnitude under both scenarios, although spatial patterns of responses differ. Projected increases in isoprene emissions (32%–94% over both countries), however, result in significantly greater changes in surface ozone. Increases of 1–15 ppb are found under A1fi and of 0–7 ppb are found under B1. These increases not only raise the frequency of “high ozone days,” but are also projected to occur nearly uniformly across the distribution of daily ozone maxima. Thus, projected future ozone changes appear to be more sensitive to changes in biogenic emissions than to direct climate changes, and the spatial patterns and magnitude of future ozone changes depend strongly on the future emissions scenarios used.

© 2015 Macmillan Publishers Limited. All rights reserved. Nearly three-quarters of the growth in global carbon emissions from the burning of fossil fuels and cement production between 2010 and 2012 occurred in China. Yet estimates of Chinese emissions remain subject to large uncertainty; inventories of China's total fossil fuel carbon emissions in 2008 differ by 0.3 gigatonnes of carbon, or 15 per cent. The primary sources of this uncertainty are conflicting estimates of energy consumption and emission factors, the latter being uncertain because of very few actual measurements representative of the mix of Chinese fuels. Here we re-evaluate China's carbon emissions using updated and harmonized energy consumption and clinker production data and two new and comprehensive sets of measured emission factors for Chinese coal. We find that total energy consumption in China was 10 per cent higher in 2000-2012 than the value reported by China's national statistics, that emission factors for Chinese coal are on average 40 per cent lower than the default values recommended by the Intergovernmental Panel on Climate Change, and that emissions from China's cement production are 45 per cent less than recent estimates. Altogether, our revised estimate of China's CO2 emissions from fossil fuel combustion and cement production is 2.49 gigatonnes of carbon (2 standard deviations = ±7.3 per cent) in 2013, which is 14 per cent lower than the emissions reported by other prominent inventories. Over the full period 2000 to 2013, our revised estimates are 2.9 gigatonnes of carbon less than previous estimates of China's cumulative carbon emissions. Our findings suggest that overestimation of China's emissions in 2000-2013 may be larger than China's estimated total forest sink in 1990-2007 (2.66 gigatonnes of carbon) or China's land carbon sink in 2000-2009 (2.6 gigatonnes of carbon).

The third affiliation in the paper was incorrect and has now been corrected to “Tyndall Centre for Climate Change Research, School of International Development, University of East Anglia, Norwich, NR4 7TJ, UK”. Furthermore, the initial of the author D. Guan has been corrected.